The 100 most-cited articles in ACS Applied Materials & Interfaces, 2018

Polydopamine is one of the simplest and most versatile approaches to functionalizing material surfaces, having been inspired by the adhesive nature of catechols and amines in mussel adhesive proteins. Since its first report in 2007, a decade of studies on polydopamine molecular structure, deposition conditions, and physicochemical properties have ensued. During this time, potential uses of polydopamine coatings have expanded in many unforeseen directions, seemingly only limited by the creativity of researchers seeking simple solutions to manipulating surface chemistry. In this review, we describe the current state of the art in polydopamine coating methods, describe efforts underway to uncover and tailor the complex structure and chemical properties of polydopamine, and identify emerging trends and needs in polydopamine research, including the use of dopamine analogs, nitrogen-free polyphenolic precursors, and improvement of coating mechanical properties.

Methacrylated gelatin (GelMA) has been widely used as a tissue-engineered scaffold material, but only low-concentration GelMA hydrogels were found to be promising cell-laden bioinks with excellent cell viability. In this work, we reported a strategy for precise deposition of 5% (w/v) cell-laden GelMA bioinks into controlled microarchitectures with high cell viability using extrusion-based three-dimensional (3D) bioprinting. By adding gelatin into GelMA bioinks, a two-step cross-linking combining the rapid and reversible thermo-cross-linking of gelatin with irreversible photo-cross-linking of GelMA was achieved. The GelMA/gelatin bioinks showed significant advantages in processability because the tunable rheology and the rapid thermo-cross-linking of bioinks improved the shape fidelity after bioprinting. Here, the rheology, mechanical properties, and swelling of GelMA/gelatin bioinks with different concentration ratios were carefully characterized to obtain the optimized bioprinting setup. We successfully printed the 5% (w/v) GelMA with 8% (w/v) gelatin into 3D structures, which had…

A hydrogel for potential applications in wound dressing should possess several peculiar properties, such as efficient self-healing ability and mechanical toughness, so as to repair muscle and skin damage. Additionally, excellent cell affinity and tissue adhesiveness are also necessary for the hydrogel to integrate with the wound tissue in practical applications. Herein, an ultratough and self-healing hydrogel with superior cell affinity and tissue adhesiveness is prepared. The self-healing ability of the hydrogel is obtained through hydrogen bonds and dynamic Schiff cross-linking between dopamine-grafted oxidized sodium alginate (OSA-DA) and polyacrylamide (PAM) chains. The covalent cross-linking is responsible for its stable mechanical structure. The combination of physical and chemical cross-linking contributes to a novel hydrogel with efficient self-healing ability (80% mechanical recovery in 6 h), high tensile strength (0.109 MPa), and ultrastretchability (2550%), which are highly desirable properties and are superior to previously reported tough and self-healing hydrogels for…

The three-dimensional (3D) printing of flexible and stretchable materials with smart functions such as shape memory (SM) and self-healing (SH) is highly desirable for the development of future 4D printing technology for myriad applications, such as soft actuators, deployable smart medical devices, and flexible electronics. Here, we report a novel ink that can be used for the 3D printing of highly stretchable, SM, and SH elastomer via UV-light-assisted direct-ink-write printing. An ink containing urethane diacrylate and a linear semicrystalline polymer is developed for the 3D printing of a semi-interpenetrating polymer network elastomer that can be stretched by up to 600%. The 3D-printed complex structures show interesting functional properties, such as high strain SM and SM -assisted SH capability. We demonstrate that such a 3D-printed SM elastomer has the potential application for biomedical devices, such as vascular repair devices. This research paves a new way for the further development of novel 4D printing, soft robotics, and biomedical devices.

Conducting polymer hydrogels (CPHs) have emerged as a fascinating class of smart soft matters important for various advanced applications. However, achieving the synergistic characteristics of conductivity, self-healing ability, biocompatibility, viscoelasticity, and high mechanical performance still remains a critical challenge. Here, we develop for the first time a type of multifunctional hybrid CPHs based on a viscoelastic polyvinyl alcohol (PVA)–borax (PB) gel matrix and nanostructured CNFs–PPy (cellulose nanofibers–polypyrrole) complexes that synergizes the biotemplate role of CNFs and the conductive nature of PPy. The CNF–PPy complexes are synthesized through in situ oxidative polymerization of pyrrole on the surface of CNF templates, which are further well-dispersed into the PB matrix to synthesize homogeneous CNF–PPy/PB hybrid hydrogels. The CNF–PPy complexes not only tangle with PVA chains though hydrogen bonds, but also form reversibly cross-linked complexes with borate ions. The multi-complexation between each component leads to the formation of a hierarchical…

Composite electrolytes are widely studied for their potential in realizing improved ionic conductivity and electrochemical stability. Understanding the complex mechanisms of ion transport within composites is critical for effectively designing high-performance solid electrolytes. This study examines the compositional dependence of the three determining factors for ionic conductivity, including ion mobility, ion transport pathways, and active ion concentration. The results show that with increase in the fraction of ceramic Li 7 La 3 Zr 2 O 12 (LLZO) phase in the LLZO–poly(ethylene oxide) composites, ion mobility decreases, ion transport pathways transit from polymer to ceramic routes, and the active ion concentration increases. These changes in ion mobility, transport pathways, and concentration collectively explain the observed trend of ionic conductivity in composite electrolytes. Liquid additives alter ion transport pathways and increase ion mobility, thus enhancing ionic conductivity significantly. It is also found that a higher content of LLZO leads to improved electrochemical…

Deep partial thickness burn wounds present big challenges due to the long healing time, large size and irregular shape, pain and reinjury at wound dressing changes, as well as scarring. The clinically effective therapy to alleviate pain at wound dressing changes, and the scar left on the skin after the healing of wound is still unavailable. To combat this, we develop a nanocomposite self-healing hydrogel that can be injected into irregular and deep burn wound beds and subsequently rapidly self-heal to reform into an integrated piece of hydrogel that thoroughly fills the wound area and protects the wound site from external environment, finally being painlessly removed by on-demand dissolving using amino acid solution at wound dressing changes, which accelerates deep partial thickness burn wound healing and prevents scarring. The hydrogel is made out of naturally occurring polymers, namely, water-soluble carboxymethyl chitosan (CMC) and rigid rod-like dialdehyde-modified cellulose nanocrystal (DACNC). They are cross-linked by dynamic Schiff-base linkages between amines from CMC and…

Integrating multifunctionality such as adhesiveness, stretchability, and self-healing ability on a single hydrogel has been a challenge and is a highly desired development for various applications including electronic skin, wound dressings, and wearable devices. In this study, a novel hydrogel was synthesized by incorporating polydopamine-coated talc (PDA-talc) nanoflakes into a polyacrylamide (PAM) hydrogel inspired by the natural mussel adhesive mechanism. Dopamine molecules were intercalated into talc and oxidized, which enhanced the dispersion of talc and preserved catechol groups in the hydrogel. The resulting dopamine-talc-PAM (DTPAM) hydrogel showed a remarkable stretchability, with over 1000% extension and a recovery rate over 99%. It also displayed strong adhesiveness to various substrates, including human skin, and the adhesion strength surpassed that of commercial double-sided tape and glue sticks, even as the hydrogel dehydrated over time. Moreover, the DTPAM hydrogel could rapidly self-heal and regain its mechanical properties without needing any external stimuli. It…

Two-dimensional (2D) MXenes have recently been shown to be promising for applications in anticancer photothermal therapy (PTT), owing to their outstanding photothermal performance. However, as with the other inorganic 2D nanomaterials, the MXene-based nanoplatforms lack the appropriate biocompatibility and stability in physiological conditions, targeting capability, and controlled release of drug, for cancer therapy. Fabricating a smart MXene-based nanoplatform for the treatment of cancer therefore remains a challenge. In this work, composite hydrogels based on cellulose and Ti 3 C 2 MXene, were synthesized for the first time. We have shown that the cellulose/MXene composite hydrogels possess rapid response near-infrared-stimulated characteristics, which present as a continuous dynamic process in water. As a result, when loaded with the anticancer drug doxorubicin hydrochloride (DOX), the cellulose/MXene hydrogels are capable of significantly accelerating the DOX release. This behavior is attributed to the expansion of the pores within the three-dimensional cellulose-based networks,…

An efficient binary Bi 2 Fe 4 O 9 /Bi 2 WO 6 Z -scheme heterojunction was fabricated through a facile hydrothermal route. The obtained Bi 2 Fe 4 O 9 /Bi 2 WO 6 displays high catalytic activity for rhodamine B (RhB) photodegradation, and 100% of RhB was photodegraded by Bi 2 Fe 4 O 9 (7%)/Bi 2 WO 6 within 90 min, which is much better than that by pure Bi 2 Fe 4 O 9 and Bi 2 WO 6 . The effective photoinduced carrier separation, the broadened photoabsorption range, high oxidation capacity of hole, and the high reduction power of electron are in charge of the elevated catalytic activity because of the formed Z -scheme system. In addition, the effects such as pollutant concentration, pH, inorganic anions, and water sources exerted on photocatalytic performance were also investigated, and the results suggest that Bi 2 Fe 4 O 9 /Bi 2 WO 6 still possesses a high photocatalytic performance. The free-radical trapping experiments and electron spin resonance spin-trapping technology disclose that hole (h + ), hydroxy radical ( • OH), and superoxide radical ( • O 2 – ) are cardinal active…

Two-dimensional (2D) particles, including transition metal carbides (MXenes), often exhibit large lateral-size polydispersity in delaminated colloidal solutions. This heterogeneity results in challenges when conducting fundamental studies, such as investigating correlations between properties and the 2D flake size. To resolve this challenge, we have developed solution-processable techniques to control and sort 2D titanium carbide (Ti 3 C 2 T x ) MXene flakes after synthesis based on sonication and density gradient centrifugation, respectively. By tuning the sonication conditions, Ti 3 C 2 T x flakes with varied lateral sizes, ranging from 0.1 to ∼5 μm, can be obtained. Furthermore, density gradient centrifugation was used to sort Ti 3 C 2 T x flakes with different lateral sizes into more monodisperse fractions. These processing techniques allow for the characterization of size-dependent optical and electronic properties by measuring the absorption spectra and film conductivity, respectively. Additionally, by testing the material as electrochemical capacitor electrodes, we show the…

Exosomes, nanoscale extracellular vesicles functioning as cell-to-cell communicators, are an emerging promising therapeutic in the field of bone tissue engineering. Here, we report the construction and evaluation of a novel cell-free tissue-engineered bone that successfully accelerated the restoration of critical-sized mouse calvarial defects through combining exosomes derived from human adipose-derived stem cells (hASCs) with poly(lactic-co-glycolic acid) (PLGA) scaffolds. The exosomes were immobilized on the polydopamine-coating PLGA (PLGA/pDA) scaffolds under mild chemical conditions. Specifically, we investigated the effects of hASC-derived exosomes on the osteogenic, proliferation, and migration capabilities of human bone marrow-derived mesenchymal stem cells in vitro and optimized their osteoinductive effects through osteogenic induction. Furthermore, an in vitro assay showed exosomes could release from PLGA/pDA scaffold slowly and consistently and in vivo results showed this cell-free system enhanced bone regeneration significantly, at least partially through its…

Electrospun nanofiber composite membranes containing water-stable metal-organic frameworks (MOFs) particles (Zr-based MOF-808) supported on polyacrylonitrile (PAN) nanofiber synthesized via co-electrospinning have been prepared. MOF particles were dispersed in the organic polymer, and their subsequent presence was inferred by scanning electron microscopy. Membrane performance in heavy metal ion adsorption in batch filtration was evaluated on the basis of Cd 2+ and Zn 2+ ions sequestration. The adsorption capacities of the pristine MOF and the MOF composite membrane revealed that MOF particles in the membrane could be accessed for adsorption in the hydrophilic PAN membranes. The maximum adsorption capacities were 225.05 and 287.06 mg g –1 for Cd 2+ and Zn 2+, respectively. Conventional thermal activation of pristine MOF and composite membrane revealed a crystal downsizing, while “hydractivation” produced an expanded MOF with enhanced adsorption potentials. The PAN/MOF-808 “hydractivated” composite membrane could treat 580 mL of Cd, whereas the conventional vacuum-activated composite…

As part of increased efforts to develop wearable healthcare devices for monitoring and managing physiological and metabolic information, stretchable electrochemical sweat sensors have been investigated. In this study, we report on the fabrication of a stretchable and skin-attachable electrochemical sensor for detecting glucose and pH in sweat. A patterned stretchable electrode was fabricated via layer-by-layer deposition of carbon nanotubes (CNTs) on top of patterned Au nanosheets (AuNS) prepared by filtration onto stretchable substrate. For the detection of glucose and pH, CoWO 4 /CNT and polyaniline/CNT nanocomposites were coated onto the CNT–AuNS electrodes, respectively. A reference electrode was prepared via chlorination of silver nanowires. Encapsulation of the stretchable sensor with sticky silbione led to a skin-attachable sweat sensor. Our sensor showed high performance with sensitivities of 10.89 μA mM –1 cm –2 and 71.44 mV pH –1 for glucose and pH, respectively, with mechanical stability up to 30% stretching and air stability for 10 days. The sensor also showed good…

It is desired to create skin strain sensors composed of multifunctional conductive hydrogels with excellent toughness and adhesion properties to sustain cyclic loadings during use and facilitate the electrical signal transmission. Herein, we prepared transparent, compliant, and adhesive zwitterionic nanocomposite hydrogels with excellent mechanical properties. The incorporated zwitterionic polymers can form interchain dipole–dipole associations to offer additional physical cross-linking of the network. The hydrogels show a high fracture elongation up to 2000%, a fracture strength up to 0.27 MPa, and a fracture toughness up to 2.45 MJ/m 3 . Moreover, the reversible physical interaction imparts the hydrogels with rapid self-healing ability without any stimuli. The hydrogels are adhesive to many surfaces including polyelectrolyte hydrogels, skin, glasses, silicone rubbers, and nitrile rubbers. The presence of abundant zwitterionic groups facilitates ionic conductivity in the hydrogels. The combination of these properties enables the hydrogels to act as strain sensors with high…

Covalently cross-linked rubbers are renowned for their high elasticity that play an indispensable role in various applications including tires, seals, and medical implants. Development of self-healing and malleable rubbers is highly desirable as it allows for damage repair and reprocessability to extend the lifetime and alleviate environmental pollution. Herein, we propose a facile approach to prepare permanently cross-linked yet self-healing and recyclable diene-rubber by programming dynamic boronic ester linkages into the network. The network is synthesized through one-pot thermally initiated thiol-ene "click" reaction between a novel dithiol-containing boronic ester cross-linker and commonly used styrene-butadiene rubber without modifying the macromolecular structure. The resulted samples are covalently cross-linked and possess relatively high mechanical strength which can be readily tailored by varying boronic ester content. Owing to the transesterification of boronic ester bonds, the samples can alter network topologies, endowing the materials with self-healing ability and…

Considerable attention has been devoted to producing antibacterial fabrics due to their very wide applications in medicine, hygiene, hospital, etc. However, the poor antibacterial durability and bad bacterial antiadhesion capacity of most existing antibacterial fabrics limit their applications. In this work, a series of antibacterial and polymeric quaternary ammonium monomers with different alkyl chain length were successfully synthesized to copolymerize with fluorine-containing and other acrylic monomers to generate cationic fluorinated polymer emulsions and durably antibacterial and bacterially antiadhesive cotton fabrics. The relation between antibacterial constituent and its antibacterial activity was investigated. The study indicated that the alkyl chain length and contents of the antibacterial monomers, as well as the add-on percentage of polymer greatly influenced the antibacterial activities of the fabrics. In addition, it was found that incorporation of fluorine component into the polymer greatly enhanced the antibacterial activity and bacterial antiadhesion of the treated…

Lightweight, ultrathin, and flexible electromagnetic interference (EMI) shielding materials with high electromagnetic shielding effectiveness (SE) and excellent mechanical robustness are greatly desired for miniaturized and highly integrated electronics. Herein, for the first time, a freestanding, ultrathin, and flexible Ti 3 C 2 T x /poly(3,4-ethylenedioxythiophene)–poly(styrenesulfonate) (PEDOT:PSS) composite film with a “brick-and-mortar” structure is biomimetically designed and fabricated via a vacuum-assisted filtration process. The ultrathin polymeric composite film with a weight ratio 7:1 of Ti 3 C 2 T x to PEDOT:PSS is only 11.1 μm in thickness but exhibits a high EMI SE value of 42.10 dB. Meanwhile, the tensile strength increases considerably from 5.62 to 13.71 MPa and the corresponding ruptured strain increases from 0.18 to 0.29% compared with pure Ti 3 C 2 T x MXene film, respectively. Moreover, the hybrid film displays a superior conductivity of 340.5 S/cm and an outstanding specific EMI shielding efficiency of 19 497.8 dB cm 2 g –1 . The superior electrical conductivity…

Water oxidation is the key process for many sustainable energy technologies containing artificial photosynthesis and metal–air batteries. Engineering inexpensive yet active electrocatalysts for water oxidation is mandatory for the cost-effective generation of solar fuels. Herein, we propose a novel hierarchical porous Ni–Co-mixed metal sulfide (denoted as NiCoS) on Ti 3 C 2 T x MXene via a metal–organic framework (MOF)-based approach. Benefiting from the unique structure and strong interfacial interaction between NiCoS and Ti 3 C 2 T x sheets, the hybrid guarantees an enhanced active surface area with prominent charge-transfer conductivity and thus a superior activity toward oxygen evolution reactions (OERs). Impressively, the hierarchical NiCoS in the hybrid is converted to nickel/cobalt oxyhydroxide–NiCoS assembly (denoted as NiCoOOH–NiCoS) by OER measurement, where NiCoOOH on the surface is confirmed as the intrinsic active species for the consequent water oxidation. The hybrid material is further applied to an air cathode for a rechargeable zinc–air battery, which exhibits low…

A variety of biomass-based carbon materials with two-level porous structure have been successfully prepared by one-step carbonization process. The first level of microscale pores templates from the inherent porous tissues, while the second one of nanopores is produced by the in situ etching by the embedded alkaline metal elements. The superimposed effect of nano and microscale pores endows the hierarchically porous carbons (HPCs) with excellent microwave absorption (MA) performance. Among them, the spinach-derived HPC exhibits a maximum reflection loss of -62.2 dB and a broad effective absorption bandwidth of 7.3 GHz. Particularly, this excellent MA performance can be reproduced using the biomass materials belonging to different families, harvested seasons, and origins, indicating a green and sustainable process. These encouraging findings shed the insights on the preparation of biomass-derived microwave absorbents with promising practical applications.

The infection of bacteria and fungus is one of the most challenging global threats to human health. With the recent advancement in nanoscience and nanotechnology, much progress has been achieved in the development of antimicrobial nanomedicine; however, these nanomaterial-based antibacterial agents still suffer from potential biological toxicity, poor degradation, and various secondary pollution. Here, we demonstrate the fabrication of low-toxic and degradable carbon dots (CDs) from vitamin C by one-step electrochemical method. These newly generated CDs display a strong broad-spectrum antibacterial activity and antifungal activity even at low concentrations, as they destroy the bacterial walls during the diffusive entrance, perturb secondary structures of DNA/RNAs of bacteria and fungus, and inhibit important gene expressions to finally kill the bacteria and fungus. We also show that these well-characterized CDs can be completely degraded into CO 2, CO and H 2 O under visible light in air (or at very mild temperature, about 37 °C).

The combination of carbon materials and ferrite materials has recently attracted increased interest in microwave absorption applications. Herein, a novel composite with cobalt cores encapsulated in a porous carbon shell was synthesized via a facile sintering process with a cobaltic metal-organic framework (Co-MOF-74) as the precursor. Because of the magnetic loss caused by the Co cores and dielectric loss caused by the carbon shell with a unique porous structure, together with the interfacial polarization between two components, the ferromagnetic composite exhibited enhanced electromagnetic wave absorption performance compared to traditional ferrite materials. With the thermal decomposition temperature of 800 °C, the optimal reflection loss value achieved -62.12 dB at 11.85 GHz with thin thickness (2.4 mm), and the bandwidth ranged from 4.1 to 18 GHz with more than 90% of the microwave that could be absorbed. The achieved performance illustrates that the as-prepared porous Co-C core-shell composite shows considerable potential as an effective microwave absorber.

Much effort has been invested for nearly five decades to identify and develop new polymer capacitor dielectrics for higher than ambient temperature applications. Simultaneous demands of processability, dielectric permittivity, thermal conductivity, and dielectric breakdown strength dictated by increasing high power performance criteria limit the number of available materials. The present review first explains the advantages of metallized polymer film capacitors over the film-foil, ceramic, and electrolytic counterparts and then presents a comprehensive review on both past developmental effort of commercial resins and recent research progress on new polymers targeted for operating temperature above 150 °C. Some historical background and discussion on the limitation of the commercially available polymer film dielectrics for high temperature applications are also given. In many cases, further development of promising polymers that appear to possess all or most of the important criteria is limited by lack of large scale market incentives but could be of great value to niche applications…

Organic materials that display thermally activated delayed fluorescence (TADF) are a striking class of functional materials that have witnessed a booming progress in recent years. In addition to pure TADF emitters achieved by the subtle manipulations of intramolecular charge transfer processes with sophisticated molecular structures, a new class of efficient TADF-based OLEDs with emitting layer formed by blending electron donor and acceptor molecules that involve intermolecular charge transfer have also been fabricated. In contrast to pure TADF materials, the exciplex-based systems can realize small Δ E ST (0–0.05 eV) much more easily since the electron and hole are positioned on two different molecules, thereby giving small exchange energy. Consequently, exciplex-based OLEDs have the prospective to maximize the TADF contribution and achieve theoretical 100% internal quantum efficiency. Therefore, the challenging issue of achieving small Δ E ST in organic systems could be solved. In this article, we summarize and discuss the latest and most significant developments regarding these…

Replacement of flammable organic liquid electrolytes with solid Li + conductors is a promising approach to realize excellent performance of Li metal batteries. However, ceramic electrolytes are either easily reduced by Li metal or penetrated by Li dendrites through their grain boundaries, and polymer electrolytes are also faced with instability on the electrode/electrolyte interface and weak mechanical property. Here, we report a three-dimensional fiber-network-reinforced bicontinuous solid composite electrolyte with flexible Li + -conductive network (lithium aluminum titanium phosphate (LATP)/polyacrylonitrile), which helps to enhance electrochemical stability on the electrode/electrolyte interface by isolating Li and LATP and suppress Li dendrites growth by mechanical reinforcement of fiber network for the composite solid electrolyte. The composite electrolyte shows an excellent electrochemical stability after 15 days of contact with Li metal and has an enlarged tensile strength (10.72 MPa) compared to the pure poly(ethylene oxide)–bistrifluoromethanesulfonimide lithium salt…

By dispersing Li 6.25 Ga 0.25 La 3 Zr 2 O 12 (Ga-LLZO) nanoparticles in poly(ethylene oxide) (PEO) matrix, PEO:Ga-LLZO composite polymer electrolytes are synthesized. The PEO: Ga-LLZO composite with 16 vol % Ga-LLZO nanoparticles shows a conductivity of 7.2 × 10 –5 S cm –1 at 30 °C, about 4 orders of magnitude higher than the conductivity of PEO. The enhancement of the ionic conductivity is closely related to the space charge region (∼3 nm) formed at the interface between the PEO matrix and the Ga-LLZO nanoparticles. The space charge region is observed by transmission electron microscope (TEM) and corroborated by the phase-field simulation. Using the random resistor model, the lithium-ion transport in the composite polymer electrolyte is simulated by the Monte Carlo simulation, demonstrating that the enhanced ionic conductivity can be ascribed to the ionic conduction in the space charge regions and the percolation of the space charge regions.

Developing convenient doping to build highly active oxygen evolution reaction (OER) electrocatalysts is a practical process for solving the energy crisis. Herein, a facile and low-cost in situ self-assembly strategy for preparing a Ce-doped NiFe-LDH nanosheets/nanocarbon (denoted as NiFeCe-LDH/CNT, LDH = layered double hydroxide and CNT = carbon nanotube) hierarchical nanocomposite is established for enhanced OER, in which the novel material provides its overall advantageous structural features, including high intrinsic catalytic activity, rich redox properties, high, flexible coordination number of Ce 3+, and strongly coupled interface. Further experimental results indicate that doped Ce into NiFe-LDH/CNT nanoarrays brings about the reinforced specific surface area, electrochemical surface area, lattice defects, and the electron transport between the LDH nanolayered structure and the framework of CNTs. The effective synergy prompts the NiFeCe-LDH/CNT nanocomposite to possess superior OER electrocatalytic activity with a low onset potential (227 mV) and Tafel slope (33 mV dec –1 ),…

Mesenchymal stem cell (MSC)-derived exosomes have been recognized as new candidates for cell-free treatment of various diseases. However, maintaining the retention and stability of exosomes over time in vivo after transplantation is a major challenge in the clinical application of MSC-derived exosomes. Here, we investigated if human placenta-derived MSC-derived exosomes incorporated with chitosan hydrogel could boost the retention and stability of exosomes and further enhance their therapeutic effects. Our results demonstrated that chitosan hydrogel notably increased the stability of proteins and microRNAs in exosomes, as well as augmented the retention of exosomes in vivo as confirmed by Gaussia luciferase imaging. In addition, we assessed endothelium-protective and proangiogenesis abilities of hydrogel-incorporated exosomes in vitro. Meanwhile, we evaluated the therapeutic function of hydrogel-incorporated exosomes in a murine model of hindlimb ischemia. Our data demonstrated that chitosan hydrogel could enhance the retention and stability of exosomes and further augment the…

MXenes, as a new family of 2D materials, can be used as film electrodes in energy storage devices because of their hydrophilic surface, metallic conductivity, and rich surface chemistries. However, the poor ion transport of MXene film electrodes causes a great loss of surface reactivity, which significantly inhibits the full exploitation of the potential of MXene-based materials. To solve this issue, we report a facile electrolyte-induced self-assembly method to construct a 3D porous structure in the MXene–rGO hybrid film, which effectively facilitates rapid diffusion and transport of electrolyte ions in the film electrode while still maintaining high electrical conductivity. When the hybrid film is employed as electrode materials for lithium-ion batteries, it exhibits high specific capacity of 335.5 mA h g –1 at 0.05 A g –1 and good rate capability of 30% capacitance retention at 4 A g –1 . Additionally, the film electrode exhibits excellent cycling stability without capacity decay after 1000 cycles under high rates (1 A g –1 ) owing to its stable structure. Furthermore, the…

All-inorganic cesium lead bromide CsPbBr 3 perovskite quantum dots (QDs) are emerging as potential candidates for their applications in optoelectronic devices but they suffer from poor long-term stability due to their high sensitivity to UV irradiation, heat, and especially to moisture. Although great advances in improving stability of perovskite QDs have been achieved by surface modification or encapsulation in polymer and silica, they are not sufficiently refrained from external environment due to nondense structures of these protective layers. In this work, in situ nanocrystallization strategy is developed to directly grow CsPbBr 3 QDs among a specially designed TeO 2 -based glass matrix. As a result, QD-embedded glass shows typical bright green emission assigned to exciton recombination radiation and significant improvement of photon/thermal stability and water resistance due to the effective protecting role of dense structural glass. Particularly, ∼90% of emission intensity is even remained after immersing QD-embedded glass in water up to 120 h, enabling them to find promising…

Immediate hemorrhage control and anti-infection play important roles in the wound management. Besides, a moist environment is also beneficial for wound healing. Hydrogels are promising materials in urgent hemostasis and drug release. However, hydrogels have the disadvantage of rapid release profiles, leading to the exposure to high drug concentrations. In this study, we constructed hybrid hydrogels with rapid hemostasis and sustainable antibacterial property combining aminoethyl methacrylate hyaluronic acid (HA-AEMA) and methacrylated methoxy polyethylene glycol (mPEG-MA) hybrid hydrogels and chlorhexidine diacetate (CHX)-loaded nanogels. The CHX-loaded nanogels (CLNs) were prepared by the enzyme degradation of CHX-loaded lysine-based hydrogels. The HA-AEMA and mPEG-MA hybrid hydrogel loaded with CLNs (labeled as Gel@CLN) displayed a three-dimensional microporous structure and exhibited excellent swelling, mechanical property, and low cytotoxicity. The Gel@CLN hydrogel showed a prolonged release period of CHX over 240 h and the antibacterial property over 10 days. The hemostasis and…

Developing high-active and low-cost bifunctional materials for catalyzing the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) holds a pivotal role in water splitting. Therefore, we present a new strategy to form NiS/Ni 2 P heterostructures. The as-obtained NiS/Ni 2 P/carbon cloth (CC) requires overpotentials of 111 mV for the HER and 265 mV for the OER to reach a current density of 20 mA cm –2, outperforming their counterparts such as NiS and Ni 2 P under the same conditions. Additionally, the NiS/Ni 2 P/CC electrode requires a 1.67 V cell voltage to deliver 10 mA cm –2 in a two-electrode electrolysis system, which is comparable to the cell using the benchmark Pt/C||RuO 2 electrode. Detailed characterizations reveal that strong electronic interactions between NiS and Ni 2 P, abundant active sites, and smaller charge-transfer resistance contribute to the improved HER and OER activity.

A new series of five three-dimensional Ln(III) metal–organic frameworks (MOFs) formulated as [Ln 4 (μ 6 -L) 2 (μ-HCOO)(μ 3 -OH) 3 (μ 3 -O)(DMF) 2 (H 2 O) 4 ] n {Ln 3+ = Tb 3+ ( 1 ), Eu 3+ ( 2 ), Gd 3+ ( 3 ), Dy 3+ ( 4 ), and Er 3+ ( 5 )} was successfully obtained via a solvothermal reaction between the corresponding lanthanide(III) nitrates and 2-(6-carboxypyridin-3-yl)terephthalic acid (H 3 L). All of the obtained compounds were fully characterized, and their structures were established by single-crystal X-ray diffraction. All products are isostructural and possess porous 3D networks of the fluorite topological type, which are driven by the cubane-like [Ln 4 (μ 3 –OH) 3 (μ 3 -O)(μ-HCOO)] 6+ blocks and μ 6 -L 3– spacers. Luminescent and sensing properties of 1 – 5 were investigated in detail, revealing a unique capability of Tb–MOF ( 1 ) for sensing acetone and metal(III) cations (Fe 3+ or Ce 3+ ) with high efficiency and selectivity. Apart from a facile recyclability after sensing experiments, the obtained Tb–MOF material features a remarkable stability in a diversity of…

Electroactive hydrogels (EAH) that exhibit large deformation in response to an electric field have received great attention as a potential actuating material for soft robots and artificial muscle. However, their application has been limited due to the use of traditional two-dimensional (2D) fabrication methods. Here we present soft robotic manipulation and locomotion with 3D printed EAH microstructures. Through 3D design and precise dimensional control enabled by a digital light processing (DLP) based micro 3D printing technique, complex 3D actuations of EAH are achieved. We demonstrate soft robotic actuations including gripping and transporting an object and a bidirectional locomotion.

Fabrication of high-performance noble-metal-free bifunctional electrocatalysts for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in water is a promising strategy toward future carbon-neutral economy. Herein, a one-pot hydrothermal synthesis of cobalt sulfide/nickel sulfide heterostructure supported by nickel foam (CoS x /Ni 3 S 2 @NF) was performed. The Ni foam acted as the three-dimensional conducting substrate as well as the source of nickel for Ni 3 S 2 . The formation of CoS x /Ni 3 S 2 @NF was confirmed by X-ray diffraction and X-ray photoelectron spectroscopy. The formation of CoS x /Ni 3 S 2 @NF facilitated easy charge transport and showed synergistic electrocatalytic effect toward HER, OER, and overall water splitting in alkaline medium. Remarkably, CoS x /Ni 3 S 2 @NF showed catalytic activity comparable with that of benchmarking electrocatalysts Pt/C and RuO 2 . For CoS x /Ni 3 S 2 @NF, overpotentials of 204 and 280 mV were required to achieve current densities of 10 and 20 mA cm –2 for HER and OER, respectively, in 1.0 M KOH solution. A…

Piezoelectric effect, commonly known as a change in electric polarization in piezoelectric/ferroelectric materials under mechanical stress, is extensively employed as a driving force for the catalytic degradation of organic pollutants. However, the relationship between electric polarization and piezocatalytic activity is still unclear. In this work, we investigated the role of ferroelectric polarization in the piezocatalytic activity of BaTiO 3 nanoparticles through annealing BaTiO 3 at different temperatures or poling BaTiO 3 at different electric fields. The BaTiO 3 nanoparticles annealed at 800 °C exhibit effectively enhanced piezocatalytic activity compared with those annealed at other temperatures. The polycrystalline particles annealed at higher temperatures exhibit a greatly reduced catalytic activity. After poling, the piezocatalytic activity of the polycrystalline BaTiO 3 particles was obviously improved. In addition, we identified the free radical species and the intermediate products of the catalytic reaction. We also well-explained the dependence of electric polarization…

Metal-organic framework (MOF)-derived porous metal/C composites have drawn considerable attention from the microwave absorption field owing to their large pore volumes and surface areas. Exploring single-MOF-derived materials with high intensity and broadband absorption is largely needed but remains a challenge. Here, porous Co/ZnO/C (CZC) microrods were fabricated easily from cuboid-shaped heterobimetallic MOFs. CZC provides an efficient platform for integrating different semiconductors (ZnO), magnetic metal (Co), and carbon sources into one particle, which enhances the electromagnetic (EM) wave-absorbing ability. The carbonization temperature which is critical for EM parameters was studied in detail. CZC annealed at 700 °C outperformed those obtained at 600 or 800 °C in terms of microwave wave-absorbing properties. The reflection loss (RL) was optimized to -52.6 (or -20.6) dB at 12.1 (or 14.8) GHz with an effective bandwidth (RL ≤ -10 dB) of 4.9 (or 5.8) GHz at the coating thickness of 3.0 (or 2.5) mm. Such enhancement of EM wave-absorbing capabilities is ascribed to the…

We investigated thermal properties of the epoxy-based composites with the high loading fraction—up to f ≈ 45 vol %—of the randomly oriented electrically conductive graphene fillers and electrically insulating boron nitride fillers. It was found that both types of the composites revealed a distinctive thermal percolation threshold at the loading fraction f T > 20 vol %. The graphene loading required for achieving thermal percolation, f T, was substantially higher than the loading, f E, for electrical percolation. Graphene fillers outperformed boron nitride fillers in the thermal conductivity enhancement. It was established that thermal transport in composites with high filler loadings, f ≥ f T, is dominated by heat conduction via the network of percolating fillers. Unexpectedly, we determined that the thermal transport properties of the high loading composites were influenced strongly by the cross-plane thermal conductivity of the quasi-two-dimensional fillers. The obtained results shed light on the debated mechanism of the thermal percolation, and facilitate the development of the…

Given their low cost and eco-friendliness, rechargeable Zn-ion batteries (ZIBs) have received increasing attention as a device with great potential for large-scale energy storage. However, the development of ZIBs with high capacities and long lifespans is challenging because of the dendritic growth of Zn and the absence of suitable cathode materials. Herein, we report a novel rechargeable aqueous Zn-ion battery (AZIB) that consist of Zn coated with reduced graphene oxide as the anode and V 3 O 7 ·H 2 O/rGO composite as the cathode. The new AZIB exhibits excellent cycle stability with a high capacity retention of 79% after 1000 cycles. Moreover, it can deliver a high power density of 8400 W kg –1 at 77 W h kg –1 and a high energy density of 186 W h kg –1 at 216 W kg –1, and the former is higher than those of previously reported AZIBs. Our work provides a new perspective in developing rechargeable ZIBs and would greatly accelerate the practical applications of rechargeable ZIBs.

The design of heterojunction with superior performance of light absorption and appropriate conduction band and valence band potentials is a promising approach for the applications in efficient environmental remediation and the solar energy storage. In recent years, many studies have been devoted to the applications of graphitic carbon nitride (g-C 3 N 4 )-based heterojunction photoactive nanomaterials under visible light irradiation due to its excellent physical, optical, and electrical properties, which inspired us to compile this review. Although many reviews demonstrated about the syntheses and applications of g-C 3 N 4 composites, a targeted review on the systematic application and photocatalytic mechanisms of g-C 3 N 4 -based heterojunction, in which components are in intimate linkage with each other rather than a physical mixture, is still absent. In this review, the applications of g-C 3 N 4 -based heterojunction photoactive nanomaterials in environmental remediation and solar energy storage, such as photocatalytic treatment of persistent organic pollutants, heavy-metal-ion…

For faster and greener anti-icing/deicing, a new generation of anti-icing materials are expected to possess both passive anti-icing properties and active deicing properties. The photothermal effect of carbon nanotubes (CNTs) is used in the field of photothermal cancer therapy, while the application in anti-icing/deicing is seldom investigated. Superhydrophobic SiC/CNTs coatings with photothermal deicing and passive anti-icing properties were first prepared by a simple spray-coating method. The results of 3D profile and microstructure observed via scanning electron microscopy demonstrate that the micronanostructure combined with peaklike SiC microstructure and villiform CNTs nanostructure makes the coatings surface superhydrophobic, exhibiting a water contact angle of up to 161° and a roll angle as low as 2°. This micronanostructure can also reduce ice anchoring and ice adhesion strength. Utilizing the photothermal effect of CNTs, the surface temperature of the coatings is rapidly increased upon near-infrared light (808 nm) irradiation. The heat is transferred rapidly to the…

A novel green synthesis strategy was proposed for preparation of multitemplate molecularly imprinted biopolymers (mt-MIBP) in aqueous media with less consumption of organic solvents, which were subsequently used as sorbents of ultrasound-assisted dispersive solid-phase extraction (d-SPE) for simultaneous recognition and efficient separation of B-family vitamins in juice samples, followed by high performance liquid chromatography (HPLC) determination. The obtained mt-MIBP was fully characterized by SEM, FT-IR, TEM, and BET. It offered high binding capacity, good selectivity, and fast dynamics toward all the templates. Involved parameters in the d-SPE efficiency such as mt-MIBP mass, sonication time, and eluting/washing solvents’ types and volumes were concurrently investigated by central composite design with rapidity and reliability. Under the optimum conditions, the developed mt-MIBP-d-SPE-HPLC method exhibited wide linear range, low limits of detection and quantification (LOQs) within 1.2–5.5 μg L –1 and 4.0–18.4 μg L –1, respectively, and appropriate repeatability (relative…

Oxygen vacancy is conducive to molecular oxygen adsorption and activation, and it is necessary to estimate its contribution on catalysts, especially the doped system for volatile organic compound (VOC) oxidation. Herein, a series of doped Mn x Zr 1– x O 2 catalysts with oxygen vacancy were prepared by partially substituting Zr 4+ in a zirconia with low-valent manganese (Mn 2+ ). Compared with the corresponding mechanically mixed samples (MB-x) without oxygen vacancy, Mn x Zr 1– x O 2 catalysts exhibited better toluene conversion and specific reaction rate, where the differential values were calculated to estimate the contribution of oxygen vacancy on catalytic performance. The increase in oxygen vacancy concentrations in Mn x Zr 1– x O 2 catalysts can boost the differential values, implying the enhancement of oxygen vacancy contribution. Density functional theory (DFT) calculations further confirmed the contribution of oxygen vacancy, and molecular oxygen is strongly absorbed and activated on a defective Mn-doped c-ZrO 2 (111) surface with oxygen vacancy rather than a perfect m-ZrO…

Nucleolus tracking and nucleus-targeted photodynamic therapy are attracting increasing attention due to the importance of nucleolus and the sensitivity of nucleus to various therapeutic stimuli. Herein, a new class of multifunctional fluorescent carbon quantum dots (or carbon dots, CDs) synthesized via the one-pot hydrothermal reaction of m-phenylenediamine and l-cysteine was reported to effectively target nucleolus. The as-prepared CDs possess superior properties, such as low-cost and facile synthesis, good water dispersibility, various surface groups for further modifications, prominent photostability, excellent compatibility, and rapid/convenient/wash-free staining procedures. Besides, as compared with SYTO RNASelect (a commonly used commercial dye for nucleolus imaging) that can only image nucleolus in fixed cells, the CDs can realize high-quality nucleolus imaging in not only fixed cells but also living cells, allowing the real-time tracking of nucleolus-related biological behaviors. Furthermore, after conjugating with protoporphyrin IX (PpIX), a commonly used photosensitizer,…

All-solid-state batteries (ASSBs) show great potential for providing high power and energy densities with enhanced battery safety. While new solid electrolytes (SEs) have been developed with high enough ionic conductivities, SSBs with long operational life are still rarely reported. Therefore, on the way to high-performance and long-life ASSBs, a better understanding of the complex degradation mechanisms, occurring at the electrode/electrolyte interfaces is pivotal. While the lithium metal/solid electrolyte interface is receiving considerable attention due to the quest for high energy density, the interface between the active material and solid electrolyte particles within the composite cathode is arguably the most difficult to solve and study. In this work, multiple characterization methods are combined to better understand the processes that occur at the LiCoO 2 cathode and the Li 10 GeP 2 S 12 solid electrolyte interface. Indium and Li 4 Ti 5 O 12 are used as anode materials to avoid the instability problems associated with Li-metal anodes. Capacity fading and increased…

Development of a high-efficiency heterojunction with an improved photocatalytic property is regarded as a promising way to decontaminate wastewater. Herein, the direct novel Z-scheme heterojunction formed between CeO 2 nanoparticles and hierarchical ZnO was synthesized through the wet chemistry method and then the heat-treatment technique. The as-synthesized ZnO/CeO 2 composites display highly enhanced photocatalytic rhodamine B (RhB) degradation compared with pristine ZnO and CeO 2 . Specifically, ZnO/CeO 2 -3 (mass fraction of CeO 2, 30%) shows good photostability and the best removal efficiency for photodegradated RhB, which are almost 2.5 and 1.7 times than pristine ZnO and CeO 2, respectively. On the basis of the detailed characterizations and the degradation behavior of as-prepared samples over RhB, the formed heterojunction between the hierarchical ZnO and CeO 2 nanoparticles is confirmed as the direct Z-scheme heterojunction. The heterojunction system shows fast transfer, high-efficiency separation, and long lifetime of photoinduced charge carriers, as well as enhanced redox…

Upconversion luminescence of nano-sized Yb 3+ and Tm 3+ codoped rare earth phosphates, that is, LaPO 4 and YPO 4, has been investigated under high-pressure (HP, up to ∼25 GPa) and high-temperature (293–773 K) conditions. The pressure-dependent luminescence properties of the nanocrystals, that is, energy red shift of the band centroids, changes of the band ratios, shortening of upconversion lifetimes, and so forth, make the studied nanomaterials suitable for optical pressure sensing in nanomanometry. Furthermore, thanks to the large energy difference (∼1800 cm –1 ), the thermalized states of Tm 3+ ions are spectrally well-separated, providing high-temperature resolution, required in optical nanothermometry. The temperature of the system containing such active nanomaterials can be determined on the basis of the thermally induced changes of the Tm 3+ band ratio ( 3 F 2,3 → 3 H 6 / 3 H 4 → 3 H 6 ), observed in the emission spectra. The advantage of such upconverting optical sensors is the use of near-infrared light, which is highly penetrable for many materials. The investigated…

Conductive hydrogels have important potential in biosensors, bioactuators, and health recording electrodes, but they are often troubled by sensitivity, operating temperature range, and whether they can be recycled or not. In this paper, conductive hydrogels poly(vinyl alcohol)/glycerol/polyaniline (PGA) were prepared by organic combination of low-cost poly(vinyl alcohol) (PVA), polyaniline (PANi), and glycerin. First, the effects of PVA, glycerol, and aniline/phytic acid solution concentration on the mechanical properties, electrical properties, and frost resistance of the PGA gel were discussed. Second, the interaction energies of PVA, PANi, phytic acid, glycerol, and water molecules were analyzed by Materials Studio. Then, a simple biosensor fabricated using the PGA gel realized the detection of the conventional motion signal of the human body. The conductive gel has high sensitivity (GF = 2.14), fast response time (230 ms), and can be circulated several times (∼540 cycles). Furthermore, the PGA conductive gel can maintain good electrical conductivity (0.32 S/m) and mechanical…

Solid-state batteries have been considered as one of the most promising next-generation energy storage systems because of their high safety and energy density. Solid-state electrolytes are the key component of the solid-state battery, which exhibit high ionic conductivity, good chemical stability, and wide electrochemical windows. LATP [Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 ] solid electrolyte has been widely investigated for its high ionic conductivity. Nevertheless, the chemical instability of LATP against Li metal has hindered its application in solid-state batteries. Here, we propose that atomic layer deposition (ALD) coating on LATP surfaces is able to stabilize the LATP/Li interface by reducing the side reactions. In comparison with bare LATP, the Al 2 O 3 -coated LATP by ALD exhibits a stable cycling behavior with smaller voltage hysteresis for 600 h, as well as small resistance. More importantly, on the basis of advanced characterizations such as high-resolution transmission electron spectroscope-electron energy loss spectroscopy, the lithium penetration into the LATP bulk and Ti…

Lightweight, stretchable, and wearable strain sensors have recently been widely studied for the development of health monitoring systems, human-machine interfaces, and wearable devices. Herein, highly stretchable polymer elastomer-wrapped carbon nanocomposite piezoresistive core-sheath fibers are successfully prepared using a facile and scalable one-step coaxial wet-spinning assembly approach. The carbon nanotube-polymeric composite core of the stretchable fiber is surrounded by an insulating sheath, similar to conventional cables, and shows excellent electrical conductivity with a low percolation threshold (0.74 vol %). The core-sheath elastic fibers are used as wearable strain sensors, exhibiting ultra-high stretchability (above 300%), excellent stability (>10 000 cycles), fast response, low hysteresis, and good washability. Furthermore, the piezoresistive core-sheath fiber possesses bending-insensitiveness and negligible torsion-sensitive properties, and the strain sensing performance of piezoresistive fibers maintains a high degree of stability under harsh conditions. On the…

Ammonia (NH 3 ) is an irritant gas with a unique pungent odor; sub-parts per million-level breath ammonia is a medical biomarker for kidney disorders and Helicobacter pylori bacteria-induced stomach infections. The humidity varies in both ambient environment and exhaled breath, and thus humidity dependence of gas-sensing characteristics is a great obstacle for real-time applications. Herein, flexible, humidity-independent, and room-temperature ammonia sensors are fabricated by the thermal evaporation of CuBr on a polyimide substrate and subsequent coating of a nanoscale moisture-blocking CeO 2 overlayer by electron-beam evaporation. CuBr sensors coated with a 100 nm-thick CeO 2 overlayer exhibits an ultrahigh response (resistance ratio) of 68 toward 5 ppm ammonia with excellent gas selectivity, rapid response, reversibility, and humidity-independent sensing characteristics at room temperature. In addition, the sensing performance remains stable after repetitive bending and long-term operation. Moreover, the sensors exhibit significant response to the simulated exhaled breath of…

Glycosaminoglycan-based hydrogels are widely used for cartilage repair because glycosaminoglycans are the main component of the cartilage extracellular matrix and can maintain chondrocyte functions. However, most of the glycosaminoglycan-based hydrogels are negatively charged and cell-repellant, and they cannot host cells or favor tissue regeneration. Inspired by mussel chemistry, we designed a polydopamine-chondroitin sulfate-polyacrylamide (PDA-CS-PAM) hydrogel with tissue adhesiveness and super mechanical properties for growth-factor-free cartilage regeneration. Thanks to the abundant reactive catechol groups on the PDA, a cartilage-specific PDA-CS complex was formed by the self-assembly of PDA and CS, and then the PDA-CS complex was homogenously incorporated into an elastic hydrogel network. This catechol-group-enriched PDA-CS complex endowed the hydrogel with good cell affinity and tissue adhesiveness to facilitate cell adhesion and tissue integration. Compared with bare CS, the PDA-CS complex in the hydrogel was more effective in exerting its functions on adhered cells to…

Constructing catalysts with new and optimizational chemical components and structures, which can operate well for both the anodic oxygen evolution reaction (OER) and the cathodic hydrogen evolution reaction (HER) at large current densities, is of primary importance in practical water splitting technology. Herein, the NiFe 2 O 4 nanoparticles/NiFe layered double hydroxide (LDH) nanosheet heterostructure array on Ni foam was prepared via a simple one-step solvothermal approach. The as-prepared heterostructure array displays high catalytic activity toward the OER with a small overpotential of 213 mV at 100 mA cm –2 and can afford a current density of 500 mA cm –2 at an overpotential of 242 mV and 1000 mA cm –2 at 265 mV. Moreover, it also presents outstanding HER activity, only needing a small overpotential of 101 mV at 10 mA cm –2, and can drive large current densities of 500 and 750 mA cm –2 at individual overpotentials of 297 and 314 mV. A two-electrode electrolyzer using NiFe 2 O 4 nanoparticles/NiFe LDH nanosheets as both the anode and the cathode implements active overall water…

All inorganic perovskite nanocrystals (NCs) of CsPbX 3 (X = Cl, Br, I, or their mixture) are regarded as promising candidates for high-performance light-emitting diode (LED) owing to their high photoluminescence (PL) quantum yield (QY) and easy synthetic process. However, CsPbX 3 NCs synthesized by the existing methods, where oleic acid (OA) and oleylamine (OLA) are generally used as surface-chelating ligands, suffer from poor stability due to the ligand loss, which drastically deteriorates their PL QY, as well as dispersibility in solvents. Herein, the OA/OLA ligands are replaced with octylphosphonic acid (OPA), which dramatically enhances the CsPbX 3 stability. Owing to a strong interaction between OPA and lead atoms, the OPA-capped CsPbX 3 (OPA-CsPbX 3 ) NCs not only preserve their high PL QY (>90%) but also achieve a high-quality dispersion in solvents after multiple purification processes. Moreover, the organic residue in purified OPA-CsPbBr 3 is only ∼4.6%, which is much lower than ∼29.7% in OA/OLA-CsPbBr 3 . Thereby, a uniform and compact OPA-CsPbBr 3 film is obtained for LED…

Synaptic transistors stimulated by light waves or photons may offer advantages to the devices, such as wide bandwidth, ultrafast signal transmission, and robustness. However, previously reported light-stimulated synaptic devices generally require special photoelectric properties from the semiconductors and sophisticated device's architectures. In this work, a simple and effective strategy for fabricating light-stimulated synaptic transistors is provided by utilizing interface charge trapping effect of organic field-effect transistors (OFETs). Significantly, our devices exhibited highly synapselike behaviors, such as excitatory postsynaptic current (EPSC) and pair-pulse facilitation (PPF), and presented memory and learning ability. The EPSC decay, PPF curves, and forgetting behavior can be well expressed by mathematical equations for synaptic devices, indicating that interfacial charge trapping effect of OFETs can be utilized as a reliable strategy to realize organic light-stimulated synapses. Therefore, this work provides a simple and effective strategy for fabricating…

Impaired wound healing in diabetics usually leads to life-threatening complications. To develop a system for fastening skin wound healing efficiently and safely in diabetics, thermos-sensitive hydrogel containing the nanodrug, loaded in the form of gelatin microspheres (GMs), was designed to deliver curcumin (Cur) as a therapeutic drug. Cur is a naturally existing polyphenolic compound with a broad range of biological functions useful for potential therapies. Because Cur molecule has weakness in both bioavailability and in vivo stability, delivery of Cur requires assistance from other molecules to act as carrier vehicles in a sustained manner for therapeutic use. At first, self-assembly of Cur nanoparticles (CNPs) was done to improve bioavailability. The CNPs were further enclosed into GMs for responding to the matrix metalloproteinases (MMPs) that usually overexpress at diabetic nonhealing wound sites. The GMs containing CNPs were loaded into the thermos-sensitive hydrogel and were finally proved for the capacity of specially induced drug release at the wound bed, which promoted…

Aqueous batteries are promising energy storage systems but are hindered by the limited selection of anodes and narrow electrochemical window to achieve satisfactory cyclability and decent energy density. Here, we design aqueous hybrid Na–Zn batteries by using a carbon-coated Zn (Zn@C) anode, 8 M NaClO 4 + 0.4 M Zn(CF 3 SO 3 ) 2 concentrated electrolyte coupled with NASICON-structured cathodes. The Zn@C anode achieves stable Zn stripping/plating and improved kinetics without Zn dendrite formation due to the porous carbon film facilitating homogeneous current distribution and Zn deposition. Furthermore, the concentrated electrolyte offers a large electrochemical window (∼2.5 V) and permits stable cycling of cathodes. As a result, the hybrid batteries exhibit extraordinary performance including high voltage, high energy density (100–150 Wh kg –1 for half battery and 71 Wh kg –1 for full battery), and excellent cycling stability of 1000 cycles.

Aqueous Zn-ion batteries, which are being proposed as large-scale energy storage solutions because of their unparalleled safety and cost advantage, are composed of a positive host (cathode) material, a metallic zinc anode, and a mildly acidic aqueous electrolyte (pH ≈ 3–7). Typically, the charge storage mechanism is believed to be reversible Zn 2+ (de)intercalation in the cathode host, with the exception of α-MnO 2, for which multiple vastly different and contradicting mechanisms have been proposed. However, our present study, combining electrochemical, operando X-ray diffraction, electron microscopy in conjunction with energy-dispersive X-ray spectroscopy, and in situ pH evolution analyses on two oxide hosts—tunneled α-MnO 2 and layered V 3 O 7 ·H 2 O vis-à-vis two nonoxide hosts—layered VS 2 and tunneled Zn 3 [Fe(CN) 6 ] 2, suggests that oxides and nonoxides follow two dissimilar charge storage mechanisms. While the oxides behave as dominant proton intercalation materials, the nonoxides undergo exclusive zinc intercalation. Stabilization of H + on the hydroxyl-terminated oxide…

In this work, we synthesized the hierarchical ZnO@C@NiO core-shell nanorods arrays (CSNAs) grown on a carbon cloth (CC) conductive substrate by a three-step method involving hydrothermal and chemical bath methods. The morphology and chemical structure of the hybrid nanoarrays were characterized in detail. The combination and formation mechanism was proposed. The conducting carbon layer between ZnO and NiO layers can efficiently enhance the electric conductivity of the integrated electrodes, and also protect the corrosion of ZnO in an alkaline solution. Compared with ZnO@NiO nanorods arrays (NAs), the NiO in CC/ZnO@C@NiO electrodes, which possess a unique multilevel core-shell nanostructure exhibits a higher specific capacity (677 C/g at 1.43 A/g) and an enhanced cycling stability (capacity remain 71% after 5000 cycles), on account of the protection of carbon layer derived from glucose. Additionally, a flexible all-solid-state supercapacitor is readily constructed by coating the PVA/KOH gel electrolyte between the ZnO@C@NiO CSNAs and commercial graphene. The energy density of this…

Solar steam generation, due to its capability of producing clean water directly by solar energy, is emerging as a promising eco-friendly and energy-efficient technology to address global challenges of water crisis and energy shortage. Although diverse materials and architectures have been explored to improve solar energy utilization, high efficiency in solar steam generation could be accomplished only with external optical and thermal management. For the first time, we report a deployable, three-dimensional (3D) origami-based solar steam generator capable of near full utilization of solar energy. This auxetic platform is designed based on Miura-ori tessellation and is able to efficiently recover radiative and convective heat loss as well as to trap solar energy via its periodic concavity pattern. The 3D solar steam generator device with a nanocarbon composite of graphene oxide and carbon nanotubes being photothermal component in this work shows a very strong dependence between its solar energy efficiency and surface areal density. The device yields an extraordinary solar energy…

Our study shows a facile two-step method which does not require the use of core templates to load a hydrophobic photosensitizer drug chlorin e6 (Ce6) within polydopamine (PDA) nanoparticles (NPs) while maintaining the intrinsic surface properties of PDA NPs. This structure is significantly different from hollow nanocapsules which are less stiff as they do not possess a core. To our knowledge, there exist no similar studies in the literature on drug loading within the polymer matrix of PDA NPs. We characterized the drug loading and release behavior of the photosensitizer Ce6 and demonstrated the therapeutic efficacy of the combined photodynamic (PDT) and photothermal therapy (PTT) from Ce6 and PDA, respectively, under a single wavelength of 665 nm irradiation on bladder cancer cells. We obtained a saturated loading amount of 14.2 ± 0.85 μM Ce6 in 1 nM PDA NPs by incubating 1 mg/mL dopamine solution with 140 μM of Ce6 for 20 h. The PDA NPs maintained colloidal stability in biological media, whereas the pi-pi (π-π) interaction between PDA and Ce6 enabled a release profile of the…

Strong EM wave absorption and lightweight are the foremost important factors that drive the real-world applications of the modern microwave absorbers. This work mainly deals with the design of highly efficient microwave absorbers, where a hierarchical carbon nanotube (CNT) forest is first grown on the carbon fiber (CF) through the catalytic chemical vapor deposition method. The hierarchical carbon nanotube grown on the carbon fiber (CNTCF) is then embedded in the epoxy matrix to synthesize lightweight nanocomposites for their use as efficient microwave absorbers. The morphological study shows that carbon nanotubes (CNTs) self-assemble to form a trapping center on the carbon fiber. The electromagnetic characteristics of resultant nanocomposites are investigated exclusively in the X-band (8.2-12.4 GHz) using the network analyzer. The synthesized nanocomposites, containing 0.35 and 0.50 wt % CNTCFs, exhibit excellent microwave absorption properties, which could be attributed to the better impedance matching conditions and high dielectric losses. The reflection loss (RL) of -42.0 dB…

Carbon dots (CDs) rank among the most promising luminescent nanomaterials for anti-counterfeiting application owing to their high fluorescence quantum yield and nontoxicity. Herein, we report a novel, high-level security performance anti-counterfeiting strategy achieved by fluorescence-lifetime-encoded CD fluorescent inks. CD-inks have identical steady-state emission properties, but they have distinctive and well-separated fluorescence lifetimes, allowing authentication of security tags using exclusively fluorescence lifetime imaging. A proof-of-concept anti-counterfeiting tag using CD-based lifetime-encoded inks is demonstrated. The developed CD lifetime-based anti-counterfeit technology is awaited to be applicable to a wide spectrum of security-protecting purposes. Furthermore, the presented method can be easily extended to integrate fluorescence-lifetime-encoded CDs in multichannel bioimaging, high-throughput flow cytometry, and optical data storage.

Electromagnetic protection in optoelectronic instruments such as optical windows and electronic displays is challenging because of the essential requirements of a high optical transmittance and an electromagnetic interference (EMI) shielding effectiveness (SE). Herein, we demonstrate the creation of an efficient transparent EMI shielding film that is composed of calcium alginate (CA), silver nanowires (AgNWs), and polyurethane (PU), via a facile and low-cost Mayer-rod coating method. The CA/AgNW/PU film with a high optical transmittance of 92% achieves an EMI SE of 20.7 dB, which meets the requirements for commercial shielding applications. A superior EMI SE of 31.3 dB could be achieved, whereas the transparent film still maintains a transmittance of 81%. The integrated efficient EMI SE and high transmittance are superior to those of most previously reported transparent EMI shielding materials. Moreover, our transparent films exhibit a highly reliable shielding ability in a complex service environment, with 98 and 96% EMI SE retentions even after 30 min of ultrasound treatment and…

Flexible pressure sensors are of great importance to be applied in artificial intelligence and wearable electronics. However, assembling a simple structure, high-performance capacitive pressure sensor, especially for monitoring the flow of liquids, is still a big challenge. Here, on the basis of a sandwich-like structure, we propose a facile capacitive pressure sensor optimized by a flexible, low-cost nylon netting, showing many merits including a high response sensitivity (0.33 kPa –1 ) in a low-pressure regime (<1 kPa), an ultralow detection limit as 3.3 Pa, excellent working stability after more than 1000 cycles, and synchronous monitoring for human pulses and clicks. More important, this sensor exhibits an ultrafast response speed (<20 ms), which enables its detection for the fast variations of a small applied pressure from the morphological changing processes of a droplet falling onto the sensor. Furthermore, a capacitive pressure sensor array is fabricated for demonstrating the ability to spatial pressure distribution. Our developed pressure sensors show great prospects in…

Recently, the biomass “bottom-up” approach for the synthesis of graphene quantum dots (GQDs) has attracted broad interest because of the outstanding features, including low-cost, rapid, and environmentally friendly nature. However, the low crystalline quality of products, substitutional doping with heteroatoms in lattice, and ambiguous reaction mechanism strongly challenge the further development of this technique. Herein, we proposed a facile and effective strategy to prepare controllable sulfur (S) doping in GQDs, occurring in a lattice substitution manner, by hydrothermal treatment of durian with platinum catalyst. S atoms in GQDs are demonstrated to exist in the thiophene structure, resulting in good optical and chemical stabilities, as well as ultrahigh quantum yield. Detailed mechanism of the hydrothermal reaction progress was investigated. High-efficiency reforming cyclization provided by platinum was evidenced by the coexistence of diversified sp 2 -fused heterocyclic compounds and thiophene derivatives. Moreover, we also demonstrated that saccharides in durian with small…

Highly Li-ion conductive Li 6 PS 5 Cl solid-state electrolytes (SSEs) were prepared by solid-state sintering method. The influence of sintering temperature and duration on the phase, ionic conductivity, and activation energy of Li 6 PS 5 Cl was systematically investigated. The Li 6 PS 5 Cl electrolyte with a high ionic conductivity of 3.15 × 10 –3 S cm –1 at room temperature (RT) was obtained by sintering at 550 °C for just 10 min, which was more efficient taking into account such a short preparation time in comparison with other reported methods to synthesize Li 6 PS 5 Cl SSEs. All-solid-state lithium sulfur batteries (ASSLSBs) based on the Li 6 PS 5 Cl SSE were assembled by using the nano-sulfur/multiwall carbon nanotube composite combined with Li 6 PS 5 Cl as the cathode and Li–In alloy as the anode. The cell delivered a high discharge capacity of 1850 mAh g –1 at RT for the first full cycle at 0.176 mA cm –2 (∼0.1C). The discharge capacity was 1393 mAh g –1 after 50 cycles. In addition, the Coulombic efficiency remained nearly 100% during galvanostatic cycling. The experimental…

Interface engineering is a key strategy to deal with the two-dimensional (2D)/three-dimensional (3D) hybrid heterostructure, since the properties of this atomic-layer-thick 2D material can easily be impacted by the substrate environment. In this work, the structural, electronic, and optical properties of the 2D/3D heterostructure of monolayer MoS 2 on wurtzite GaN surface without and with nitridation interfacial layer are systematically investigated by first-principles calculation and experimental analysis. The nitridation interfacial layer can be introduced into the 2D/3D heterostructure by remote N 2 plasma treatment to GaN sample surface prior to stacking monolayer MoS 2 on top. The calculation results reveal that the 2D/3D integrated heterostructure is energetically favorable with a negative formation energy. Both interfaces demonstrate indirect band gap, which is a benefit for longer lifetime of the photoexcited carriers. Meanwhile, the conduction band edge and valence band edge of the MoS 2 side increases after nitridation treatment. The modification to band alignment is then…

Three-dimensional (3D) printing technologies are emerging as an important tool for the manufacturing of electrodes for various electrochemistry applications. It has been previously shown that metal 3D electrodes, modified with metal oxides, are excellent catalysts for various electrochemical energy and sensing applications. However, the metal 3D printing process, also known as selective laser melting, is extremely costly. One alternative to metal-based electrodes for the aforementioned electrochemical applications is graphene-based electrodes. Nowadays, the printing of polymer-/graphene-based electrodes can be carried out in a matter of minutes using cheap and readily available 3D printers. Unfortunately, these polymer/graphene electrodes exhibit poor electrochemical activity in their native state. Herein, we report on a simple activation method for graphene/polymer 3D printed electrodes by a combined solvent and electrochemical route. The activated electrodes exhibit a dramatic increase in electrochemical activity with respect to the [Fe(CN) 6 ] 4–/3– redox couple and the hydrogen…

Soft, flexible, and stretchable electronics are needed to transmit power and information, and track dynamic poses in next-generation wearables, soft robots, and biocompatible devices. Liquid metal has emerged as a promising material for these applications due to its high conductivity and liquid phase state at room temperature; however, surface oxidation of liquid metal gives it unique behaviors that are often incompatible with scalable manufacturing techniques. This paper reports a rapid and scalable approach to fabricate soft and flexible electronics composed of liquid metal. Compared to other liquid metal patterning approaches, this approach has the advantages of compatibility with a variety of substrates, ease of scalability, and efficiency through automated processes. Nonconductive liquid metal nanoparticle films are sintered into electrically conductive patterns by use of a focused laser beam to rupture and ablate particle oxide shells, and allow their liquid metal cores to escape and coalesce. The laser sintering phenomenon is investigated through comparison with focused ion…

Efficient rare earth elements (REEs) separation and recovery are crucial to meet the ever-increasing demand for REEs extensively used in various high technology devices. Herein, we synthesized a highly stable chromium-based metal–organic framework (MOF) structure, Cr-MIL-101, and its derivatives with different organic functional groups (MIL-101-NH 2, MIL-101-ED (ED: ethylenediamine), MIL-101-DETA (DETA: diethylenetriamine), and MIL-101-PMIDA (PMIDA: N -(phosphonomethyl)iminodiacetic acid)) and explored their effectiveness in the separation and recovery of La 3+, Ce 3+, Nd 3+, Sm 3+, and Gd 3+ in aqueous solutions. The prepared materials were characterized using various analytical instrumentation. These MOFs showed increasing REE adsorption capacities in the sequence MIL-101 < MIL-101-NH 2 < MIL-101-ED < MIL-101-DETA < MIL-101-PMIDA. MIL-101-PMIDA showed superior REE adsorption capacities compared to other MOFs, with Gd 3+ being the element most efficiently adsorbed by the material. The adsorption of Gd 3+ onto MIL-101-PMIDA was examined in detail as a function of the solution pH,…

Graphyne and its family are new carbon allotropes in 2D form with both sp and sp 2 hybridization. Recently, the graphyne with different structures have attracted great attentions from both experimental and theoretical communities, especially because the first successful synthesis of graphdiyne, which is a typical member of the graphyne family. In this review, recent theoretical progresses in the research of the graphyne family are summarized. More specifically, we systematically introduce the structural, mechanical, band, electronic transport, and thermal properties of graphyne and its family, as well as their possible applications, such as gas separation, water desalination and purification, anode material for ion battery, H 2 storage, and catalysis application. Several related theoretical methods are also reviewed. The coexistence of sp and sp 2 hybridization and the unique atom arrangement of the graphyne family members bring many novel properties and make them promising materials for many potential applications.

Molybdenum disulfide (MoS 2 ), as a promising gas-sensing material, has gained intense interest because of its large surface-to-volume ratio, air stability, and various active sites for functionalization. However, MoS 2 -based gas sensors still suffer from low sensitivity, slow response, and weak recovery at room temperature, especially for NO 2 . Fabrication of heterostructures may be an effective way to modulate the intrinsic electronic properties of MoS 2 nanosheets (NSs), thereby achieving high sensitivity and excellent recovery properties. In this work, we design a novel p–n hetero-nanostructure on MoS 2 NSs using interface engineering via a simple wet chemical method. After surface modification with zinc oxide nanoparticles (ZnO NPs), the MoS 2 /ZnO hetero-nanostructure is endowed with an excellent response (5 ppm nitrogen dioxide, 3050%), which is 11 times greater than that of pure MoS 2 NSs. To the best of our knowledge, such a response value is much higher than the response values reported for MoS 2 gas sensors. Moreover, the fabricated hetero-nanostructure also improves…

Highly efficient electromagnetic shielding materials entailing strong electromagnetic wave absorption and low reflection have become an increasing requirement for next-generation communication technologies and high-power electronic instruments. In this study, a new strategy is employed to provide flexible waterborne polyurethane composite films with an ultra-efficient electromagnetic shielding effectiveness (EMI SE) and low reflection by constructing gradient shielding layers with a magnetic ferro/ferric oxide deposited on reduced graphene oxide (rGO@Fe 3 O 4 ) and silver-coated tetraneedle-like ZnO whisker (T-ZnO/Ag) functional nanoparticles. Because of the differences in density between rGO@Fe 3 O 4 and T-ZnO/Ag, a gradient structure is automatically formed during the film formation process. The gradient distribution of rGO@Fe 3 O 4 over the whole thickness range forms an efficient electromagnetic wave absorption network that endows the film with a strong absorption ability on the top side, while a thin layer of high-density T-ZnO/Ag at the bottom constructs a highly conductive…

Current treatment approaches for spinal cord injuries (SCIs) are mainly based on cellular transplantation. Induced pluripotent stem cells (iPSCs) without supply constraints and ethical concerns have emerged as a viable treatment option for repairing neurological disorders. However, the primarily limitations in the neuroregeneration field are uncontrolled cell differentiation, and low cell viability caused by the ischemic environment. The mechanical property of three-dimensional (3D) hydrogel can be easily controlled and shared similar characteristics with nerve tissue, thus promoting cell survival and controlled cell differentiation. We propose the combination of a 3D gelatin methacrylate (GelMA) hydrogel with iPSC-derived NSCs (iNSCs) to promote regeneration after SCI. In vitro, the iNSCs photoencapsulated in the 3D GelMA hydrogel survived and differentiated well, especially in lower-moduli hydrogels. More robust neurite outgrowth and more neuronal differentiation were detected in the soft hydrogel group. To further evaluate the in vivo neuronal regeneration effect of the GelMA…

This paper demonstrates a facile and low-cost carbothermal reduction preparation of monodisperse Fe 3 O 4 /C core–shell nanosheets (NSs) for greatly improved microwave absorption. In this protocol, the redox reaction between sheet-like hematite (α-Fe 2 O 3 ) precursors and acetone under inert atmosphere and elevated temperature generates Fe 3 O 4 /C core–shell NSs with the morphology inheriting from α-Fe 2 O 3 . Thus, Fe 3 O 4 /C core–shell NSs of different sizes ( a ) and Fe 3 O 4 /C core–shell nanopolyhedrons are obtained by using different precursors. Benefited from the high crystallinity of the Fe 3 O 4 core and the thin carbon layer, the resultant NSs exhibit high specific saturation magnetization larger than 82.51 emu·g –1 . Simultaneously, the coercivity enhances with the increase of a, suggesting a strong shape anisotropy effect. Furthermore, because of the anisotropy structure and the complementary behavior between Fe 3 O 4 and C, the as-obtained Fe 3 O 4 /C core–shell NSs exhibit strong natural magnetic resonance at a high frequency, enhanced interfacial polarization, and…

Flexible and wearable pressure sensor may offer convenient, timely, and portable solutions to human motion detection, yet it is a challenge to develop cost-effective materials for pressure sensor with high compressibility and sensitivity. Herein, a cost-efficient and scalable approach is reported to prepare a highly flexible and compressible conductive sponge for piezoresistive pressure sensor. The conductive sponge, poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS)@melamine sponge (MS), is prepared by one-step dip coating the commercial melamine sponge (MS) in an aqueous dispersion of poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS). Due to the interconnected porous structure of MS, the conductive PEDOT:PSS@MS has a high compressibility and a stable piezoresistive response at the compressive strain up to 80%, as well as good reproducibility over 1000 cycles. Thereafter, versatile pressure sensors fabricated using the conductive PEDOT:PSS@MS sponges are attached to the different parts of human body; the capabilities of these devices to detect a…

Abstract The high Li-ion conductivity of the argyrodite Li6PS5Cl makes it a promising solid electrolyte candidate for all-solid-state Li-ion batteries. For future application, it is essential to identify facile synthesis procedures and to relate the synthesis conditions to the solid electrolyte material performance. Here, a simple optimized synthesis route is investigated that avoids intensive ball milling by direct annealing of the mixed precursors at 550 °C for 10 h, resulting in argyrodite Li6PS5Cl with a high Li-ion conductivity of up to 4.96 × 10–3 S cm–1 at 26.2 °C. Both the temperature-dependent alternating current impedance conductivities and solid-state NMR spin–lattice relaxation rates demonstrate that the Li6PS5Cl prepared under these conditions results in a higher conductivity and Li-ion mobility compared to materials prepared by the traditional mechanical milling route. The origin of the improved conductivity appears to be a combination of the optimal local Cl structure and its homogeneous distribution in the material. All-solid-state cells consisting of an 80Li2S–20LiI…

Electrode materials with high surface area, tailored pore size, and efficient capability for ion insertion and enhanced transport of electrons and ions are needed for advanced supercapacitors. In the present study, a mixed metal–organic framework (MOF) (cobalt- and manganese-based MOF) was synthesized through a simple one-pot solvothermal method and employed as the electrode material for the supercapacitor. Notably, a Co–Mn MOF electrode displayed a large surface area and excellent cycling stability (over 95% capacitance retention after 1500 cycles). Also, superior pseudocapacitive behavior was observed for the Co–Mn MOF electrode in the KOH electrolyte with an exceptional areal capacitance of 1.318 F cm –2 . Moreover, an asymmetric supercapacitor was assembled using Co–Mn MOF and activated carbon electrode as positive and negative electrodes, respectively. The fabricated supercapacitor showed a specific capacitance of 106.7 F g –1 at a scan rate of 10 mV s –1 and delivered a maximum energy density of 30 W h kg –1 at 2285.7 W kg –1 . Our studies suggest the Co–Mn MOF as promising…

Today’s materials research aims at excellent mechanical performance in combination with advanced functionality. In this regard, great progress has been made in tailoring the materials by assembly processes in bottom-up approaches. In the field of wood-derived materials, nanocellulose research has gained increasing attention, and materials with advanced properties were developed. However, there are still unresolved issues concerning upscaling for large-scale applications. Alternatively, the sophisticated hierarchical scaffold of wood can be utilized in a top-down approach to upscale functionalization, and one can profit at the same time from its renewable nature, CO 2 storing capacity, light weight, and good mechanical performance. Nevertheless, for bulk wood materials, a wider multipurpose industrial use is so far impeded by concerns regarding durability, natural heterogeneity as well as limitations in terms of functionalization, processing, and shaping. Here, we present a novel cellulose bulk material concept based on delignification and densification of wood resulting in a…

Developing cost-effective and highly efficient bifunctional electrocatalysts for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is of great interest for overall water splitting but still remains a challenging issue. Herein, a self-template route is employed to fabricate a unique hybrid composite constructed by encapsulating cobalt nitride (Co 5.47 N) nanoparticles within three-dimensional (3D) N-doped porous carbon (Co 5.47 N NP@N-PC) polyhedra, which can be served as a highly active bifunctional electrocatalyst. To afford a current density of 10 mA cm –2, the as-fabricated Co 5.47 N NP@N-PC only requires overpotentials as low as 149 and 248 mV for HER and OER, respectively. Moreover, an electrolyzer with Co 5.47 N NP@N-PC electrodes as both the cathode and anode catalyst in alkaline solutions can drive a current density of 10 mA cm –2 at a cell voltage of only 1.62 V, superior to that of the Pt/IrO 2 couple. The excellent electrocatalytic activity of Co 5.47 N NP@N-PC can be mainly ascribed to the high inherent conductivity and rich nitrogen vacancies of…

Effective bone regeneration remains a challenge for bone-tissue engineering. In this study, we propose a new strategy to accelerate bone regeneration via a sustained supply of phosphorus without providing foreign calcium. Herein, a black phosphorus nanosheet (BPN)-based hydrogel platform was developed, and the BPNs were used to stably and mildly provide phosphorus. The hydrogel was fabricated by photo-crosslinking of gelatin methacrylamide, BPNs, and cationic arginine-based unsaturated poly(ester amide)s. This platform combines the following advantages: the hydrogel scaffold would keep BPNs inside, and the encapsulated BPNs can degrade into phosphorus ions and capture calcium ions to accelerate biomineralization in a bone defect. The introduction of BPNs helped to enhance the mechanical performance of hydrogels, photoresponsively release phosphate, and accelerate mineralization in vitro. Moreover, BPN-containing hydrogels improved osteogenic differentiation of human dental pulp stem cells via the bone morphogenic protein-runt-related transcription factor 2 pathway. In vivo results…

Eutectic gallium-indium alloy (EGaIn) liquid metal is highly conductive, moldable, and extremely deformable and has attracted significant attention for many applications, ranging from stretchable electronics to drug delivery. Even though EGaIn liquid metal is generally known to have low toxicity, the toxicity of the metal, rather than a salt form of Ga or In, has not been systematically studied yet. In this paper, we investigate the time-dependent concentration of the ions released from EGaIn liquid metal in an aqueous environment and their cytotoxicity to human cells. It is observed that only the Ga ion is dominantly released from EGaIn when no external agitation is applied, whereas the concentration of the In ion drastically increases with sonication. The cytotoxicity study reveals that all human cells tested are viable in the growth media with naturally released EGaIn ions, but the cytotoxicity becomes significant with sonication-induced EGaIn releasates. On the basis of the comparative study with other representative toxic elements, that is, Hg and Cd, it could be concluded that…

We present the first cell-attachable and visible-light-crosslinkable bioinks based on gelatin methacryloyl (GelMA) with eosin Y (EY) photoinitiation for stereolithography three-dimensional (3D) bioprinting. To develop a visible-light-crosslinkable hydrogel, we systematically studied five combinations of GelMA and EY photoinitiator with various concentrations. Their mechanical properties, microstructures, and cell viability and confluency after encapsulation were investigated rigorously to elucidate the effects of the EY and GelMA macromer concentrations on the characteristics of the hydrogel. Experimental results show that the compressive Young's modulus and pore size are positively affected by the concentration of EY, whereas the mass swelling ratio and cell viability are negatively affected. Increasing the concentration of GelMA helps in improving the compressive Young's modulus and cell attachment. We further employed the developed visible-light-based stereolithography bioprinting system to print the patterned cell-laden hydrogels to demonstrate the bioprinting applications of…

Dichromate is known for severe health impairments to organisms. New and valid strategies have been developed to rapidly detect and efficiently remove this pollutant. Constructing stable luminescent metal-organic frameworks (MOFs) for dichromate recognition and removal from aqueous solution could provide a feasible resolution to this problem. Herein, a new luminescent Zr(IV)-MOF, Zr 6 O 4 (OH) 7 (H 2 O) 3 (BTBA) 3 (BUT-39, BUT = Beijing University of Technology) was constructed through the reaction of a newly designed functionalized T-shaped ligand 4,4′,4″-(1 H -benzo[ d ]imidazole-2,4,7-triyl)tribenzoic acid (H 3 BTBA) with zirconium salt. BUT-39 has a unique porous framework structure, in which Zr 6 cluster acts as a rare low-symmetric 9-connected node and BTBA 3– as a T-shaped 3-connected linker. As far as we know, this represents the first case of a (3,9)-connected Zr(IV)-MOF. BUT-39 could retain its framework integrity in boiling water, 2 M HCl aqueous solution, and pH 12 NaOH aqueous solution. Due to its good water stability and strong fluorescent emission, BUT-39 is then…

Conductive hydrogels (CHs) have gained significant attention for their wide applications in biomedical engineering owing to their structural similarity to soft tissues. However, designing CHs that combine biocompatibility with good mechanical and electrical properties is still challenging. Herein, we report a new strategy for the fabrication of tough CHs with excellent conductivity, superior mechanical properties, and good biocompatibility by using chitosan framework as molecular templates for controlling conducting polypyrrole (PPy) nanorods in situ formation inside the hydrogel networks. First, polyacrylamide/chitosan (CS) interpenetrating polymer network hydrogel was synthesized by UV photopolymerization; second, hydrophobic and conductive pyrrole monomers were absorbed and fixed on CS molecular templates and then polymerized with FeCl 3 in situ inner hydrophilic hydrogel network. This strategy ensured that the hydrophobic PPy nanorods were uniformly distributed and integrated with the hydrophilic polymer phase to form highly interconnected conductive path in the hydrogel,…

A series of flexible, lightweight, and highly conductive cellulose nanopapers were fabricated through in situ polymerization of aniline monomer on to cellulose nanofibers with a rationale for attenuating electromagnetic radiations within 8.2-12.4 GHz (X band). The demonstrated paper exhibits good conductivity due to the formation of a continuous coating of polyaniline (PANI) over the cellulose nanofibers (CNF) during in situ polymerization, which is evident from scanning electron microscopy, Fourier transform infrared spectroscopy, and X-ray diffraction analysis. The free hydroxyl groups on the surface of nanocellulose fibers promptly form intermolecular hydrogen bonding with PANI, which plays a vital role in shielding electromagnetic radiations and makes the cellulose nanopapers even more robust. These composite nanopapers exhibited an average shielding effectiveness of ca. -23 dB (>99% attenuation) at 8.2 GHz with 1 mm paper thickness. The fabricated papers exhibited an effective attenuation of electromagnetic waves by a predominant absorption mechanism (ca. 87%) rather than…

Copper oxides have been of considerable interest as electrocatalysts for CO 2 reduction (CO2R) in aqueous electrolytes. However, their role as an active catalyst in reducing the required overpotential and improving the selectivity of reaction compared with that of polycrystalline copper remains controversial. Here, we introduce the use of selected-ion flow tube mass spectrometry, in concert with chronopotentiometry, in situ Raman spectroscopy, and computational modeling, to investigate CO2R on Cu 2 O nanoneedles, Cu 2 O nanocrystals, and Cu 2 O nanoparticles. We show experimentally that the selective formation of gaseous C 2 products (i.e., ethylene) in CO2R is preceded by the reduction of the copper oxide (Cu 2 OR) surface to metallic copper. On the basis of density functional theory modeling, CO2R products are not formed as long as Cu 2 O is present at the surface because Cu 2 OR is kinetically and energetically more favorable than CO2R.

Photocatalytic CO 2 conversion into solar fuels has an alluring prospect. However, the rapid recombination of photogenerated electron–hole pairs for TiO 2 -based photocatalyst hinders its wide application. To alleviate this bottleneck, a ternary hybrid TiO 2 –MnO x –Pt composite is excogitated. Taking advantage of the surface junction between {001} and {101} facets, MnO x nanosheets and Pt nanoparticles are selectively deposited on each facet by a facile photodeposition method. This design accomplishes the formation of two heterojunctions: p–n junction between MnO x and TiO 2 {001} facet and metal–semiconductor junction between Pt and TiO 2 {101} facet. Both of them, together with the surface heterojunction between {001} and {101} facets, are contributive to the spatial separation of the photogenerated electron–hole pairs. Thanks to their cooperative and synergistic effect, the as-prepared composite photocatalyst exhibits a promoted yield of CH 4 and CH 3 OH, which is over threefold of pristine TiO 2 nanosheets films. The conjecture of the mechanism that selective formation of…

Microwave absorption is a critical challenge with progression in electronics, where fine structural designing of absorbent materials plays an effective role in optimizing their microwave absorption properties. Here, we have developed Fe 3 O 4 @C (FC) and Fe–Fe 3 O 4 @C (FFC) hybrid nanorings via a hydrothermal method coupled with a chemical catalytic vapor deposition technique. FC and FFC hybrid nanorings have fine carbon coating while their size can easily be tunable in a certain range from 80–130 to 90–140 nm. The optimized FC and FFC hybrid nanorings bear minimum reflection loss (RL) values of −39.1 dB at 15.9 GHz and −32.9 dB at 17.1 GHz, respectively, whereas FFC shows an effective absorption bandwidth (RL values < −10 dB) ranged from 5.2 to 18 GHz. Such an enhanced microwave absorption performance of hybrid nanorings is mainly due to the suitable impedance characteristics, multilevel interfaces, and polarization features in nanorings. This work provides an approach to design hybrid materials having a complex structure to enhance the microwave absorption properties.

As a next-generation high-power lighting technology, laser lighting has attracted great attention in high-luminance applications. However, thermally robust and highly efficient color converters suitable for high-quality laser lighting are scarce. Despite its versatility, the phosphor-in-glass (PiG) has been seldom applied in laser lighting because of its low thermal conductivity. In this work, we develop a unique architecture in which a phosphor-in-glass (PiG) film was directly sintered on a high thermally conductive sapphire substrate coated by one-dimensional photonic crystals. The designed color converter with the composite architecture exhibits a high internal quantum efficiency close to that of the original phosphor powders and an excellent packaging efficiency up to 90%. Furthermore, the PiG film can even be survived under the 11.2 W mm –2 blue laser excitation. Combining blue laser diodes with the YAG-PiG-on-sapphire plate, a uniform white light with a high luminance of 845 Mcd m –2 (luminous flux: 1839 lm), luminous efficacy of 210 lm W –1, and correlated color temperature…

Strain sensors that are capable of monitoring complex human motions with high accuracy are highly desirable for developing wearable electronics. This paper reports the fabrication of highly stretchable and sensitive multidirectional strain sensors with tunable strain gauge factors by employing a digitally controlled printer to incorporate carbon nanotube (CNT) layers into polydimethylsiloxane (PDMS) substrates. The fabricated sensors exhibit a high stretchability (up to 45%) and sensitivity with a gauge factor of 35.75. The gauge factors could be easily modulated by tuning the number of CNT printing cycles to accommodate diverse requirements. The cyclic loading-unloading test results revealed that the composite strain sensors exhibited excellent long-term durability. Particularly, in this work, for the first time, human-motion-induced strain was measured by a motion capture system and compared with the strain data obtained from the fabricated strain sensors. The deviation of strains measured by composite sensors is less than 20%, indicating the great accuracy of CNT/PDMS sensors to…

Magnetic metal nanostructures have exhibited good electromagnetic wave (EMW) absorption properties. However, the surface of the nanostructures is easily oxidized upon exposure to air, leading to the bad stability of the EMW absorption properties. We use metal-organic framework structure as a template to fabricate hollow N-doped carbon polyhedron containing CoNi alloy nanoparticles embedded within N-doped graphene (CoNi@NG-NCPs). The atomic ratio of Co/Ni can be tuned from 1:0.54 to 1:0.91 in the hollow CoNi@NG-NCPs. Experimental results demonstrate that the EMW absorption properties of the CoNi@NG-NCPs can be improved through the Ni introduction and increased with an increase of the Ni content. Typically, the minimal reflection loss of the optimal CoNi@NG-NCP can reach -24.03 dB and the effective absorption bandwidth (reflection loss below -10 dB) is as large as 4.32 GHz at the thickness of 2.5 mm. Furthermore, our CoNi@NG-NCPs exhibit favorably comparable or superior EMW absorption properties to other magnetic absorbers. In addition, because the CoNi alloy nanoparticles are coated…

Designable electromagnetic parameters accompanied by a low density of metal–organic framework (MOF)-derived metal/carbon composites are essential prerequisites for excellent microwave-absorbing materials. However, the conventional route is confined to slight modification of the physicochemical properties of metal species and carbon, which also restricts the functionalization of MOF-derived materials. Here, a facile technique has been improved by making full use of highly porous structure to uniformly introduce metallic Co nanoparticles into carbon matrix derived from Cu 3 (btc) 2 . Through changing the starting amount of Co sources, the composition of the final products can be tuned, offering an effective route to control electromagnetic properties. Multiple attenuation mechanisms are employed to realize excellent reflection loss performance, which can be clarified by modified equivalent circuit mode. Effective frequency bandwidth ( f e ) over the whole X band can be obtained by optimizing interfacial polarization through changing interface area and electrical conductivity. Broad f…

The further development of lithium–sulfur (Li–S) batteries is limited by the fact that the soluble polysulfide leads to the shuttle effect, thereby reducing the cycle stability and cycle life of the batteries. To address this issue, here a thin and lightweight (8 μm and 0.24 mg cm –2 ) reduced graphene oxide@MoS 2 (rGO@MoS 2 ) interlayer between the cathode and the commercial separator is developed as a polysulfide barrier. The rGO plays the roles of both a polysulfide physical barrier and an additional current collector, while MoS 2 has a high chemical adsorption for polysulfides. The experiments demonstrate that the Li–S cell constructed with an rGO@MoS 2 -coated separator shows a high reversible capacity of 1122 mAh g –1 at 0.2 C, a low capacity fading rate of 0.116% for 500 cycles at 1 C, and an outstanding rate performance (615 mAh g –1 at 2 C). Such an interlayer is expected to be ideal for lithium–sulfur battery applications because of its excellent electrochemical performance and simple synthesis process.

Perovskite oxide is an attractive low-cost alternative catalyst for oxygen evolution reaction (OER) relative to the precious metal oxide-based electrocatalysts (IrO 2 and RuO 2 ). In this work, a series of Sr-doped La-based perovskite oxide catalysts with compositions of La 1– x Sr x FeO 3−δ ( x = 0, 0.2, 0.5, 0.8, and 1) are synthesized and characterized. The OER-specific activities in alkaline solution increase in the order of LaFeO 3−δ (LF), La 0.8 Sr 0.2 FeO 3−δ (LSF-0.2), La 0.5 Sr 0.5 FeO 3−δ (LSF-0.5), SrFeO 3−δ (SF), and La 0.2 Sr 0.8 FeO 3−δ (LSF-0.8). We establish a direct correlation between the enhancement in the specific activity and the amount of surface oxygen vacancies as well as the surface Fe oxidation states. The improved specific activity for LSF-0.8 is clearly linked to the optimum amount of surface oxygen vacancies and surface Fe oxidation states. We also find that the OER performance stability is a function of the crystal structure and the deviation in the surface La and/or Sr composition(s) from their bulk stoichiometric compositions. The cubic structure and…

The construction of a Z-scheme heterojunction is an effective way to isolate photogenerated electron–holes and enhance the activity of the semiconductor photocatalysts. However, the Z-scheme heterojunctions based on metal–organic frameworks were rarely reported. Herein, a novel oxygen-defective ZnO (O-ZnO)/reduced graphene oxide (rGO)/UiO-66-NH 2 Z-scheme heterojunction has been prepared by a facile solvothermal route. The morphologies, structures, and photoelectric characteristics of the acquired materials were characterized in detail. The photocatalytic activity of the O-ZnO/rGO/UiO-66-NH 2 heterostructure was assessed by photocatalytic CO 2 reduction. The results indicated that the O-ZnO/rGO/UiO-66-NH 2 heterostructure could efficiently reduce CO 2 to CH 3 OH and HCOOH, and its activity was significantly superior to that of O-ZnO/UiO-66-NH 2 and ZnO/rGO/UiO-66-NH 2 . Under illumination of visible light, the yield of CH 3 OH and HCOOH over the O-ZnO/rGO/UiO-66-NH 2 heterostructure reached 34.83 and 6.41 μmol g –1 h –1, respectively. The high photoactivity of the…

Highly sensitive and stable gas sensors have attracted much attention because they are the key to innovations in the fields of environment, health, energy savings and security, etc. Sensing materials, which influence the practical sensing performance, are the crucial parts for gas sensors. Metal–organic frameworks (MOFs) are considered as alluring sensing materials for gas sensors because of the possession of high specific surface area, unique morphology, abundant metal sites, and functional linkers. Herein, four kinds of porous hierarchical Co 3 O 4 structures have been selectively controlled by optimizing the thermal decomposition (temperature, rate, and atmosphere) using ZIF-67 as precursor that was obtained from coprecipitation method with the co-assistance of cobalt salt and 2-methylimidazole in the solution of methanol. These hierarchical Co 3 O 4 structures, with controllable cross-linked channels, meso-/micropores, and adjustable surface area, are efficient catalytic materials for gas sensing. Benefits from structural advantages, core–shell, and porous core–shell Co 3 O 4…

Gas formation caused by parasitic side reactions is one of the fundamental concerns in state-of-the-art lithium-ion batteries because gas bubbles might block local parts of the electrode surface, hindering lithium transport and leading to inhomogeneous current distributions. Here, we elucidate on the origin of CO 2, which is the dominant gaseous species associated with the layered lithium nickel cobalt manganese oxide (NCM) cathode, by implementing isotope labeling and electrolyte substitution in differential electrochemical mass spectrometry–differential electrochemical infrared spectroscopy measurements. Li 2 CO 3 on the NCM surface was successfully labeled with 13 C via a process that involves its removal followed by intentional growth. In situ gas analytics on such NCM samples with 13 C-labeled Li 2 CO 3 clearly indicate that Li 2 CO 3 decomposition contributes to CO 2 evolution, especially during the first charge. At the same time, the greater contribution of electrolyte decomposition was indicated by the large amount of 12 CO 2 observed. Employment of butyronitrile as the…

The neuromorphic system processes enormous information even with very low energy consumption, which practically can be achieved with photonic artificial synapse. Herein, a photonic artificial synapse is demonstrated based on an all-oxide highly transparent device. The device consists of conformally grown In 2 O 3 /ZnO thin films on a fluorine-doped tin oxide/glass substrate. The device showed a loop opening in current–voltage characteristics, which was attributed to charge trapping/detrapping. Ultraviolet illumination-induced versatile features such as short-term/long-term plasticity and paired-pulse facilitation were truly confirmed. Further, photonic potentiation and electrical habituation were implemented. This study paves the way to develop a device in which current can be modulated under the action of optical stimuli, serving as a fundamental step toward the realization of low-cost synaptic behavior.