The 100 most-cited articles in Chemical Communications, 2023

Biomarkers are essential in biology, physiology, and pharmacology; thus, their detection is of extensive importance.

Covalent organic frameworks (COFs) are porous and crystalline organic polymers, which have found usage in various fields. These frameworks are tailorable through the introduction of diverse functionalities into the platform. Indeed, functionality plays a key role in their different applications. However, sometimes functional groups are not compatible with reaction conditions or can compete and interfere with other groups of monomers in the direct synthetic method. Also, pre-synthesis of bulky moieties in COFs can negatively affect crystal formation. To avoid these problems a post-synthetic modification (PSM) approach is a helpful tactic. Also, with the assistance of this strategy porous size can be tunable and stability can be improved without considerable effect on the crystallite. In addition, conductivity, hydrophobicity/ hydrophilicity, and chirality are among the features that can be reformed with this method. In this review, different types of PSM strategies based on recent articles have been divided into four categories: (i) post-functionalization, (ii) post-metalation, (iii)…

Organic room-temperature phosphorescence (RTP) materials are currently the focus of research in the field of bioimaging. In comparison with the conventional imaging modalities based on organic fluorescent dyes, RTP materials with long lifetime enable time-resolved imaging to improve the imaging resolution by avoiding autofluorescence. In this review, we will start with summarizing strategies for achieving high performance RTP materials for bioimaging, including the development of RTP-compounds, host-guest doping materials, and supramolecular assemblies. We then discuss the optimization of nanonization processes to obtain RTP nanoparticles with controllable size, high dispersibility, and improved stability. The differences between top-down and bottom-up approaches are further described. Finally, we briefly introduce the emerging methods for preparing RTP materials for bioimaging.

for MR-TADF materials with some supportive strategies including extending charge delocalization, heavy atom introduction, multi-donor/acceptor utilization, and a hyperfluorescence system approach. Furthermore, the outlook and prospects for future developments in MR-TADF skeletons are described.

This review introduces recent advances of covalent triazine framework-based materials for electrochemical energy storage and conversion, including supercapacitors, alkali-ion batteries, lithium–sulfur batteries, HER, ORR/OER, and carbon dioxide reduction reaction.

) due to the large energy gap and small spin-orbit coupling values between singlet and triplet excited states. In order to optimize the RISC process, strategies such as heavy-atom-integration, metal perturbation, π-conjugation extension and peripheral decoration of donor/acceptor units have been proposed to construct efficient MR-TADF materials for high-performance OLEDs. This article provides an overview of the recent progress in MR-TADF emitters with an efficient RISC process, focusing on the structure-activity relationship between the molecular structure, optoelectronic feature, and OLED performance. Finally, the potential challenges and future prospects of MR-TADF materials are discussed to gain a more comprehensive understanding of the opportunities for efficient narrowband OLEDs.

are two types of MXene materials that have been widely studied in the field of electrocatalysis. At present, research on the synthesis of MXenes is focused on carbides, whereas research on nitrides is rare, and there are no synthesis methods meeting the requirements of green, safety, high efficiency and industrialization simultaneously. Therefore, it is very important to explore environmentally friendly industrial production routes and devote more research efforts to the synthesis of MXene nitrides.

Vacancies are ubiquitous in nature, usually playing an important role in determining how a material behaves, both physically and chemically. As a consequence, researchers have introduced oxygen, sulphur and other vacancies into bi-dimensional (2D) materials, with the aim of achieving high performance electrodes for electrochemical energy storage. In this article, we focused on the recent advances in vacancy engineering of 2D materials for energy storage applications (supercapacitors and secondary batteries). Vacancy defects can effectively modify the electronic characteristics of 2D materials, enhancing the charge-transfer processes/reactions. These atomic-scale defects can also serve as extra host sites for inserted protons or small cations, allowing easier ion diffusion during their operation as electrodes in supercapacitors and secondary batteries. From the viewpoint of materials science, this article summarises recent developments in the exploitation of vacancies (which are surface defects, for these materials), including various defect creation approaches and cutting-edge…

CASSCF/RASSI-SO methods have played a prominent role in estimating various spin Hamiltonian parameters and establishing the mechanism of magnetization relaxation in this class of molecules. Particularly, various strategies to quench QTM effects go hand-in-hand with experiments, and different methods proposed to quell QTM effects are scattered in the literature. In this perspective, we have explored various approaches that are proposed in the literature to quench QTM effects, and these include the role of (i) local symmetry of lanthanides, (ii) super-exchange interaction in {3d-4f} complexes, (iii) direct-exchange interaction in {radical-4f} and metal-metal bonded complexes to suppress the QTM, (iv) utilizing external stimuli such as an electric field or pressure to modulate the QTM and (v) avoiding QTM effects by stabilising toroidal states in 4f and {3d-4f} clusters. We believe the strategies summarized here will help to design new-generation SMMs.

Discovering efficient photocatalysts has long been the goal of photocatalysis, which has traditionally been driven by serendipitous or try-and-error strategies. Recent developments in photocatalysis integrated with machine learning techniques promise to accelerate the discovery of photocatalysts, but are also facing significant challenges. In this review, advances in machine learning integrated photocatalysis are first presented from the perspective of three main photocatalytic processes: light harvesting, charge generation and separation, and surface redox reactions. Next, progress in using machine learning to understand complex photoactivity-structure relationships and identify the factors governing activity follows. A future photocatalysis paradigm is then provided with the integration of artificial intelligence, robots and automation. Lastly, we discuss the current challenges in machine learning integrated photocatalysis. This review aims to provide a systematic overview and guidelines to the broad scientific community interested in photocatalysis and artificial intelligence for…

Metal-organic frameworks (MOFs, also known as porous coordination polymers or PCPs) are a novel class of crystalline porous material. The tailorable porous structure, in terms of size, geometry and function, has attracted the attention of researchers across all disciplines of materials science. One of the many exciting aspects of MOFs is that through directional and reversible coordination bonding, organic linkers (chromophores with metal-coordinating functional groups) and metal ions (and clusters) can be spatially organized in a preconceived geometry. The well-defined spatial geometry of the metals and linkers is very advantageous for optoelectronic functions (solar cells, light-emitting diodes, photocatalysts) of the materials. This feature article evaluates the scope of charge transfer (CT) interactions in MOFs, involving the organic linkers and metal ion or cluster components. Irrespective of the type (size, shape, electronic property) of organic chromophores involved, MOFs provide an insightful path to design and make the CT process efficient. The selected examples of MOFs…

Recently, Zr- and Ti-based metal-organic frameworks (MOFs) have gathered increasing interest in the field of chemistry and materials science, not only for their ordered porous structure, large surface area, and high thermal and chemical stability, but also for their various potential applications. Particularly, the unique features of Zr- and Ti-based MOFs enable them to be a highly versatile platform for catalysis. Although much effort has been devoted to developing Zr- and Ti-based MOF materials, they still suffer from difficulties in targeted synthesis, especially for Ti-based MOFs. In this Feature Article, we discuss the evolution of Zr- and Ti-based MOFs, giving a brief overview of their synthesis and structures. Furthermore, the catalytic uses of Zr- and Ti-based MOF materials in the previous 3-5 years have been highlighted. Finally, perspectives on the Zr- and Ti-based MOF materials are also proposed. This work provides in-depth insight into the advances in Zr- and Ti-based MOFs and boosts their catalytic applications.

Considering the recent rapid advancement of synthetic technologies promoted by visible light in the last 15 years, the use of photocatalysts has been rightfully justified based on the fact that organic molecules generally do not absorb visible light. However, an increasing number of different classes of organic molecules is being identified as actually directly absorbing in this region of the electromagnetic spectrum. Among them, diazo compounds are possibly one of these classes whose chemistry has been more explored so far. Indeed, irradiation of these compounds with visible light has been introduced as a mild photolytic strategy generally leading to free carbene intermediates. This strategy not only allows for a more cost-economical approach revealing similar outcomes to some previously reported thermal, metal-catalyzed transformations; but it can also eventually lead to different reactivities. Herein, we will present the contributions of our laboratory and of other groups to this research area, along with some important elements of design behind the development of selected…

Axially chiral styrenes, a type of atropisomer analogous to biaryls, have attracted great interest because of their unique presence in natural products and asymmetric catalysis. Since 2016, a number of methodologies have been developed for the atroposelective construction of these chiral skeletons, involving both transition metal catalysis and organocatalysis. In this feature article, we aim to provide a comprehensive understanding of recent advances in the asymmetric synthesis of axially chiral styrenes catalyzed by transition metals, integrating scattered work with different catalytic systems together. This feature article is cataloged into five sections according to the strategies, including asymmetric coupling, enantioselective C-H activation, central-to-axial chirality transfer, asymmetric alkyne functionalization, and atroposelective [2+2+2] cycloaddition.

This Feature Article simply introduces principles and mechanisms of electrochemiluminescence (ECL) biosensors for the determination of biomarkers and highlights recent advances of ECL biosensors on key aspects including new ECL reagents and materials, new biological recognition elements, and emerging construction biointerfacial strategies with illustrative examples and a critical eye on pitfalls and discusses challenges and perspectives of ECL biosensors for health analysis.

Lignin is an aromatic heteropolymer, found in plant cell walls as 20-30% of lignocellulose. It represents the most abundant source of renewable aromatic carbon in the biosphere, hence, if it could be depolymerised efficiently, then it would be a highly valuable source of renewable aromatic chemicals. However, lignin presents a number of difficulties for biocatalytic or chemocatalytic breakdown. Research over the last 10 years has led to the identification of new bacterial enzymes for lignin degradation, and the use of metabolic engineering to generate useful bioproducts from microbial lignin degradation. The aim of this article is to discuss the chemical mechanisms used by lignin-degrading enzymes and microbes to break down lignin, and to describe current methods for generating aromatic bioproducts from lignin using enzymes and engineered microbes.

no solvent?" This review focuses on a three-part answer to that question: when there is little change ("solvent-optional" reactions); when solvent needs to be present in some form, even if only in the amounts provided by liquid-assisted (LAG) or solvate-assisted grinding; and those cases in which mechanochemistry allows access to compounds that cannot be obtained from solution-based routes. The emphasis here is on inorganic and organometallic systems, including selected examples of mechanosynthesis and mechanocatalysis. Issues of mechanochemical depictions and the adequacy of LAG descriptions are also reviewed.

nanosurface energy transfer (NSET) or Förster resonance energy transfer (FRET) offers powerful ways of tuning and amplifying optical signals and is relatively common, metal-QD nanohybrids for plasmon-enhanced fluorescence (PEF) have been much less prevalent. A major reason is the competition between fluorescence quenching and enhancement, which poses important challenges for optimizing distances, orientations, and spectral overlap toward maximum PEF. In this feature article, we discuss the interplay of the different quenching and enhancement mechanisms (a mixed distance dependence of quenching and enhancement - "quenchancement") to better understand the obstacles that must be overcome for the development of metal-QD nanohybrid-based PEF biosensors. The different nanomaterials, their combination within various surface and solution based design concepts, and their structural and photophysical characterization are reviewed and applications toward advanced optical biosensing and bioimaging are presented along with guidelines and future perspectives for sensitive, selective, and…

In recent years, with the development of organic synthetic chemistry, a variety of organic synthetic methods have been discovered and applied in practical production. Photochemistry and electrochemistry have been widely used in organic synthesis recently due to their advantages such as mild conditions and green and environmental protection and have now been developed into two of the most massive synthetic strategies in the field of organic synthesis. In order to further enhance the potential of photochemistry and electrochemistry and to overcome the limitations of each, organic synthetic chemists have worked to combine the two synthetic strategies together to develop photoelectrochemistry as a new synthetic method. Photoelectrochemistry achieves the complementary advantages and disadvantages of photochemistry and electrochemistry, avoids the problem of using stoichiometric oxidants or reductants in photochemistry and easy dimerization in electrochemistry, generates highly reactive reaction intermediates under mild conditions, and achieves reactions that are difficult to accomplish…

Pyrolysis-free metal-organic frameworks (MOFs) with optimized particle sizes were used as capacitive deionization (CDI) materials in oxygenated saline water. Upon decreasing the particle size of the MOFs, excellent cycling stability and higher CDI performance were achieved. This was possibly due to the improvement in charge transfer and electrolyte permeation, uncovering the significance of particle size control in improving CDI performance.

Covalent organic frameworks (COFs) are constructed exclusively with lightweight organic scaffolds, which can have a 2D or 3D architecture. The ease of synthesis, robust skeleton and tunable properties of COFs make them superior candidates among their counterparts for a wide range of uses including biomedical applications. In the biomedical field, drug delivery or photodynamic-photothermal (PDT-PTT) therapy can be individually considered a potential parameter to be investigated. Therefore, this comprehensive review is focused on drug delivery using COFs, highlighting the encapsulation and decapsulation of drugs by COF scaffolds and their delivery in biological media including live cells. Versatile COF scaffolds together with the delivery of several drug molecules are considered. We attempted to incorporate the status of drug encapsulation and decapsulation considering a wide range of recent publications.

Development of circularly polarized luminescence (CPL) materials utilizing supramolecular strategies has recently attracted increasing interest in supramolecular chemistry and materials science. Chiral macrocycles, especially chiral macrocyclic hosts, have stable structures, adjustable internal cavities to encapsulate different guests, and host-guest complexation to induce special photophysical properties. Consequently, various CPL materials based on chiral macrocycles have been developed during the last decade. To gain a better understanding of this rapidly developing research area, it is necessary and also important to summarize the advances in CPL materials based on chiral macrocycles. In this review, CPL materials from different chiral macrocycles, especially classical and newly reported chiral macrocyclic hosts and their derivatives, will be comprehensively summarized. It is believed that this review will be of guiding significance and also very helpful for the development of macrocyclic chemistry and CPL materials.

The activation and transformation of organic chemical bonds is a fundamental scientific problem. In the past several decades, C-S bond cleavage for the construction of C-C and C-heteroatom bonds has received tremendous attention in organic chemistry. Although significant progress has been made in the field of transition metal strategies, a variety of novel transition-metal-free strategies have also been developed using halogenated reagents, oxidants, acids, and bases. Moreover, organic photochemical and electrochemical methods have also been developed to achieve transition-metal-free C-S bond cleavage of organosulfur compounds. To date, however, no comprehensive review of transition-metal-free strategies has been reported. Therefore, we herein provide a comprehensive review of the major advances in the field of the transition-metal-free C-S bond cleavage and transformation of organosulfur compounds, including thioethers, sulfoxides, sulfones, thioacetals, sulfonium salts, and sulfur ylides.

Although alkynes are one of the smallest functional groups, they are among the most versatile building blocks for organic chemistry, with applications ranging from biochemistry to material sciences. Alkynylation reactions have traditionally relied on the use of acetylenes as nucleophiles. The discovery and development of ethynyl hypervalent iodine reagents have allowed to greatly expand the transfer of alkynes as electrophilic synthons. In this feature article the progress in the field since 2018 will be presented. After a short introduction on alkynylation reactions and hypervalent iodine reagents, the developments in the synthesis of alkynyl hypervalent iodine reagents will be discussed. Their recent use in base-mediated and transition-metal catalyzed alkynylations will be described. Progress in radical-based alkynylations and atom-economical transformations will then be presented.

), which are 1.9 and 22 times higher than those of pure CN, respectively. This improvement primarily results from hydrogen bonding (H-bonding) between CN and MCC, which enables excellent charge separation and migration, leading to the outstanding photoelectrochemical properties of MCC-0.05/CN.

Fluorescence microscopy has revolutionised our understanding of biological systems, enabling the visualisation of biomolecular structures and dynamics in complex systems. The possibility to reversibly control the optical or biochemical properties of fluorophores can unlock advanced applications ranging from super-resolution microscopy to the design of multi-stimuli responsive and functional biosensors. In this Highlight, we review recent progress in small-molecule photoswitches applied to biological imaging with an emphasis on molecular engineering strategies and promising applications, while underlining the main challenges in their design and implementation.

In the field of molecular magnetism, the lanthanide-radical (Ln-Rad) method has become one of the most appealing tactics for introducing strong magnetic interactions and has spurred on the booming development of heterospin single-molecule magnets (SMMs). The article is a timely retrospect on the research progress of Ln-Rad heterospin systems and special attention is invested on low dimensional Ln-Rad compounds with SMM behavior, primarily concerning with nitrogen-based radicals, semiquinone and nitroxide radicals. Rational design, molecular structures, magnetic behaviors and magneto-structural correlations are highlighted. Meanwhile, particular attention is focused on the influence of exchange couplings on the dynamic magnetic properties, with the purpose of helping to guide the design of prospective radical-based Ln-SMMs.

) as well as low cost. However, the problems of fast voltage/capacity fading, poor rate performance and the low initial Coulombic efficiency severely hinder its practical application. In this paper, we review the latest research advances of LRMO cathode materials, including crystal structure, electrochemical reaction mechanism, existing problems and modification strategies. In this review, we pay more attention to recent progress in modification methods, including surface modification, doping, morphology and structure design, binder and electrolyte additives, and integration strategies. It not only includes widely studied strategies such as composition and process optimization, coating, defect engineering, and surface treatment, but also introduces many relatively novel modification methods, such as novel coatings, grain boundary coating, gradient design, single crystal, ion exchange method, solid-state batteries and entropy stabilization strategy. Finally, we summarize the existing problems in the development of LRMO and put forward some perspectives on the further research.

The site-selective modification of amino acids, peptides, and proteins has always been an intensive topic in organic synthesis, medicinal chemistry, and chemical biology due to the vital role of amino acids in life. Among the developed methods, the site-selective introduction of fluorine functionalities into amino acids and peptides has emerged as a useful approach to change their physicochemical and biological properties. With the increasing demand for life science, the direct fluorination/fluoroalkylation of proteins has also received increasing attention because of the unique properties of fluorine atom(s) that can change the protein structure, increase their lipophilicity, and enable fluorine functionality as a biological tracer or probe for chemical biology studies. In this feature article, we summarized the recent advances in the synthesis of fluorinated amino acids and peptides, wherein two strategies have been discussed. One is based on the fluorinated building blocks to prepare fluorinated amino acids and peptides with diversified structures, including the transformations…

Electrocatalytic direct seawater splitting is considered to be one of the most desirable and necessary approach to produce substantial amount of green hydrogen to meet the energy demand. However, practical seawater splitting remains far-fetched due to the electrochemical interference of multiple elements present in seawater, among which chlorine chemistry is the most aggravating one, causing severe damages to electrodes. To overcome such limitations, apart from robust electrocatalyst design, electrolyte engineering along with in depth corrosion engineering are essential aspects, which needs to be thoroughly judged and explored. Indeed, extensive studies and various approaches including smart electrolyzer design have been attempted in the last couple of years on this matter. The present review offers a comprehensive discussion on various strategies to achieve effective and sustainable direct seawater splitting, avoiding chlorine electrochemistry to achieve industry-level performances.

Benefitting from the favorable mass diffusion kinetics and increased exposed active sites, the amorphous Fe–Co oxide shows satisfactory UOR and HER performance in alkaline seawater.

In this review article, we have highlighted the recent advancements in the design of fluorescence chemosensors for sensing ammonia both in the solution and vapor phases.

, second-harmonic generation and circularly polarized luminescence. Here, we discuss the pioneering reports on multifunctional materials that use luminescent lanthanide SMMs, with the emphasis of our contribution relying on the functionalization of 4f metal complexes through their insertion into heterometallic d-f coordination compounds.

The excessive use of traditional fossil fuels has led to energy and environmental pollution problems. Solar-driven hydrogen generation has attracted much attention in recent years owing to its environmental friendliness and economic feasibility. So far, a series of photocatalysts have been advanced. Unfortunately, these photocatalysts face some issues including poor sunlight harvesting ability, weak photo-corrosion resistance, broad band gap, bad stability, inferior hydrogen evolution rate and so on. It just so happens that COFs have emerged to provide an opportunity for settling these issues. Covalent organic frameworks (COFs), a novel family of porous materials with regular porosity and tunable physicochemical structures, have been extensively explored as photocatalysts for hydrogen production. Moreover, their photocatalytic activities are highly structurally dependent. In this review, we mainly focus on the linkage chemistry and disparate strategies for boosting COF-based photocatalytic hydrogen generation performance in detail. The prospects and obstacles confronted in the…

The fabrication of metal halide perovskite films using the solvent-engineering method is increasingly common. In this method, the crystallisation of the perovskite layer is triggered by the application of an antisolvent during the spin-coating of a perovskite precursor solution. Herein, we introduce the current state of understanding of the processes involved in the crystallisation of perovskite layers formed by solvent engineering, focusing in particular on the role of antisolvent properties and solvent-antisolvent interactions. By considering the impact of the Hansen solubility parameters, we propose guidelines for selecting the appropriate antisolvent and outline open questions and future research directions for the fabrication of perovskite films by this method.

There is an urgent need for cleaner production processes for chemicals. An efficient and promising alternative for such reactions is heterogeneous photocatalysis, which works on the principle of converting (visible) light, including solar energy, into chemical energy. To that end, properly designed semiconductor based photocatalysts are necessary to trigger the photocatalytic reactions. Many commonly used photocatalysts have too large bandgaps (3-3.4 eV) to use visible light and a too low surface area for efficient production. Metal-organic frameworks (MOFs) have emerged as an encouraging class of materials for photocatalytic applications due to their (i) large surface area and porosity that facilitate adsorption towards chemicals, (ii) tunable crystallinity and optical and electronic properties for efficient light absorption in the visible region, (iii) tunable composition and functionality that make them versatile photocatalysts for a wide range of reactions, and (iv) facile development of composites with other semiconductors to produce Z-scheme heterojunctions that can…

Tetracoordinate boron compounds are a highly important class of molecules, which are the key intermediates in many organoboron-related chemical transformations and have unique luminescence properties. However, the synthesis of tetracoordinate boron compounds has never been reviewed. In this highlight, we summarize recent progress on the construction of racemic and chiral tetracoordinate borons, and hope to provide ideas for the assembly of them in more efficient ways, especially for the construction of boron-stereogenic compounds.

evolution, and nitrate reduction. Additionally, the advances and shortages of BBS applied in these processes are summarized and comprehensively discussed. Future works for BBS applied in photoreduction processes are also proposed.

The electrochemical interfacial interaction of electrode materials with liquid electrolytes in electrochemical energy storage systems including supercapacitors, metal ion batteries, and metal-based batteries have become a research hotspot and play a decisive role in electrochemical energy storage in terms of charging and discharging reaction principles of the electrode materials. However, there is still a long way from maturity due to the challenges related to the unsatisfactory electrolyte-philicity of electrode materials. In the last 20 years, several studies have been directed at discovering strategies to improve the electrolyte-philicity of electrode materials, optimizing the electrochemical interfacial interaction of the electrode materials with liquid electrolytes and exploring the relationship between electrolyte-philicity and electrochemical energy storage performance in the charging and discharging processes of the electrode materials. Unfortunately, the systematic and in-depth understanding of electrolyte-philicity of electrode materials has not been grasped in…

With natural ilmenite as the heterogeneous photocatalyst, ferrocene and air as the homogeneous redox-catalysts, H-bonds as the promoter, and EtOH/H 2 O as the solvent, a semi-heterogeneous decarboxylative annulation of quinoxalin-2(1 H )-ones was developed.

Photoelectrochemical (PEC) water splitting for hydrogen evolution has been considered as a promising technology to solve the energy and environmental issues. However, the solar-to-hydrogen (STH) conversion efficiencies of current PEC systems are far from meeting the commercial demand (10%) due to the lack of efficient photoelectrode materials. The recent rapid development of defect engineering of photoelectrodes has significantly improved the PEC performance, which is expected to break through the bottleneck of low STH efficiency. In this review, the category and the construction methods of different defects in photoelectrode materials are summarized. Based on the in-depth summary and analysis of existing reports, the PEC performance enhancement mechanism of defect engineering is critically discussed in terms of light absorption, carrier separation and transport, and surface redox reactions. Finally, the application prospects and challenges of defect engineering for PEC water splitting are presented, and the future research directions in this field are also proposed.

Zinc ferrite based nanostructures for magnetic hyperthermia applications.

pH-responsive systems have gained importance for the development of smart materials and for biomedical applications because they can switch between different states by simple acid/base triggers. However, such equilibrium systems lack the autonomous behaviour that is so ubiquitous in living systems that self-regulate out of equilibrium. As a contribution to the emerging field of autonomous chemical systems, we have developed pH-feedback systems (pH-FS) based on the coupling of acid- and base-producing steps in chemical reaction networks. The resulting autonomous nonlinear pH curves can be coupled with a variety of pH-sensitive building blocks to program the lifecycles of the associated transient state at the level of self-assemblies and material systems. In this article, we discuss the different generations of such pH-feedback systems, the principles of their coupling to self-assemblies with lifecycles and highlight emerging concepts for the design of autonomous functional materials. The specificity, robustness, and flexible operation of such pH-FS can also be used to realize…

ontology. Thus, the proposed catalysts informatics would help innovate how catalysts can be designed and understood.

= 242 °C) indicate that it can be used as a melt-cast explosive. The novelty, synthetic feasibility, and energetic performance of all the molecules suggest that they can be used as potential secondary explosives in defence and civilian fields.

Heterogeneous catalysis is an important class of reactions in industrial production, especially in green chemical synthesis, and environmental and organic catalysis. Single-atom catalysts (SACs) have emerged as promising candidates for heterogeneous catalysis, due to their outstanding catalytic activity, high selectivity, and maximum atomic utilization efficiency. The high specific surface energy of SACs, however, results in the migration and aggregation of isolated atoms under typical reaction conditions. The controllable preparation of highly efficient and stable SACs has been a serious challenge for applications. Herein, we summarize the recent progress in the precise synthesis of SACs and their different heterogeneous catalyses, especially involving the oxidation and reduction reactions of small organic molecules. At the end of this review, we also introduce the challenges confronted by single-atom materials in heterogeneous catalysis. This review aims to promote the generation of novel high-efficiency SACs by providing an in-depth and comprehensive understanding of the current…

Hydrogen production through alkaline water electrolysis holds great promise as a scalable solution for renewable energy storage and conversion. The development of non-precious metal-based electrocatalysts with low-overpotential for alkaline water electrolysis is essential to decrease the cost of electrolysis devices. Although the Ni-based and Fe-based electrocatalysts have been commercially employed in the cathodic hydrogen evolution reaction (HER) and anodic oxygen evolution reaction (OER), it is imperative to persistently pursue the advancement of highly efficient electrocatalysts with enhanced current density and fast kinetics. This feature article overviews the progress of NiMo HER cathodes and NiFe OER anodes in the traditional alkaline water electrolysis process for hydrogen production, including the detailed mechanisms, preparation strategies, and structure-function relationship. Moreover, recent advances of Ni-based and Fe-based electrodes in the process of novel alkaline water electrolysis, involving small energetic molecule electro-oxidation and redox mediator decoupled…

Halogenated organic compounds are widespread, and decades of heavy use have resulted in global bioaccumulation and contamination of the environment, including water sources. Here, we introduce the most common halogenated organic water pollutants, their classification by type of halogen (fluorine, chlorine, or bromine), important policies and regulations, main applications, and environmental and human health risks. Remediation techniques are outlined with particular emphasis on carbon-halogen bond strengths. Aqueous advanced redox processes are discussed, highlighting mechanistic details, including electrochemical oxidations and reductions of the water-oxygen system, and thermodynamic potentials, protonation states, and lifetimes of radicals and reactive oxygen species in aqueous electrolytes at different pH conditions. The state of the art of aqueous advanced redox processes for brominated, chlorinated, and fluorinated organic compounds is presented, along with reported mechanisms for aqueous destruction of select PFAS (per- and polyfluoroalkyl substances). Future research…

A metal–organic-framework-based Li + ion trap was designed via tailoring linker functionality as well as free –COOH density.

A Cu nanoparticle-decorated TiO 2 nanobelt array on a titanium plate acts as a catalyst for NH 3 electrosynthesis via NO 2 − reduction, attaining an NH 3 yield of 760.5 μmol h −1 cm −2 (237.7 μmol h −1 mg cat. −1 ) and a high Faradaic efficiency of 95.3%.

Oxidative stress denotes the imbalance between the generation of reactive oxygen species (ROS) and antioxidant defenses in living organisms, participating in various pathophysiological processes and mediating the occurrence of diseases. Typically, the excessive production of ROS under oxidative stress elicits oxidative modification of biomacromolecules, including lipids, proteins and nucleic acids, leading to cell dysfunction and damage. Therefore, the analysis and detection of oxidative stress-associated biomarkers are of considerable importance to accurately reflect and evaluate the oxidative stress status. This review comprehensively elucidates the recent advances and applications of imaging probes for tracking and detecting oxidative stress-related biomarkers such as lipid peroxidation, and protein and DNA oxidation. The existing challenges and future development directions in this field are also discussed.

various C-C and C-heteroatom bond-forming reactions. The advantages of these approaches include (i) use of feedstock chemicals, (ii) high atom economy, (iii) no pre-activation of the substrates, and (iv) producing water as the only by-product. In this context, several synthetic strategies have been developed in this regime for the past few decades. To the best of our knowledge, no review article describes the important concepts of interrupted borrowing hydrogen (IBH) reaction. This review article highlights the recent advances in the IBH strategy and its application in sustainable chemical synthesis, particularly C-C bond formation using methanol as a C1 source, synthesis of 3,3'-bisindolylmethanes (3,3'-BIMs), α-branched ketones/diketones, and regioselective alkylation of N-heterocycles.

> 4) have seen major advances in recent years. Fundamental properties originating from their high atomic number (such as the size, energy, and polarizability of atomic orbitals) set them apart from more established species in small molecule activation. Challenges and opportunities arising from this scenario are analyzed and highlighted.

Complex mixtures are ubiquitous in many branches of chemistry, be it a complex pharmaceutical formulation, a collection of biofluids analysed in a metabolomics workflow, or a flowing mixture in a reaction monitoring setting. The accurate quantitative determination of mixture components is one of the toughest challenges posed to analytical chemists, requiring the determination of often heavily overlapped signals from compounds in very diverse concentrations. NMR spectroscopists have developed an impressive variety of approaches to deal with such challenges, including the development of innovative pulse sequences, hyperpolarization methods and processing tools. We describe the most recent advances in the field of quantitative NMR, and the many subsequent application perspectives in fields where the sample complexity is a daily challenge, such as pharmaceutical science, metabolomics, isotopic analysis, and monitoring.

Copper-catalyzed decarboxylative reactions of propargylic cyclic carbonates/carbamates enable the efficient construction of widely available skeletons such as allenes, ethynyl-containing heterocycles, and tetrasubstituted stereogenic carbon centers. As an emerging field, these strategies have gained great attention and shown significant progress due to the presence of multiple electrophilic and nucleophilic reaction sites of propargylic cyclic carbonates/carbamates, as well as the distinct advantages of copper catalysis such as higher selectivity, low cost, and mild reaction conditions. In this review, the achievements in copper-catalyzed decarboxylative reactions of propargylic cyclic carbonates/carbamates are addressed. Mechanistic insights, synthetic applications, and their limitations are discussed. The challenges and opportunities of this field are also outlined.

As a class of promising cathodes in the field of large-scale power storage systems especially for alkali-metal-ion batteries (MIBs), Prussian blue (PB) and its analogues (PBAs) have received wide research attention due to their open framework, high theoretical specific capacity, and simple synthesis method. For large-scale applications, cathode materials with low-cost and long cycle life are preferred. However, only a few of the review papers have concentrated on the detailed analysis of low-cost PBAs, including Fe-based and Mn-based PBAs, which also show excellent electrochemical performance. This review aims to first provide an all-sided understanding of low-cost PBAs in terms of their application and recent progress in MIBs. Then, the major challenges such as inferior electrochemical properties of low-cost PBAs are discussed. Meanwhile, we provide feasible strategies to prepare PBA electrodes with advanced electrochemical performance. Finally, we present some personal perspectives and guidance for future research, aiming to narrow the gap between laboratory investigation and…

Hydrogen production from electrocatalytic water splitting driven by renewable energy sources provides a promising path for energy sustainability. The current water electrolysis technologies mainly use fresh water as feedstock, which will further aggravate the shortage of water resources in the world. Seawater has an innate advantage in large-scale electrolysis hydrogen production because of its abundant reserves. However, direct seawater electrolysis without any pre-treatment faces serious challenges due to the electrode side reactions and corrosion issues caused by the complex compositions of seawater. In this review, we first discuss the basic principles of seawater electrolysis. Second, the recent progress in designing efficient direct seawater electrolysis systems is discussed in detail, including catalyst design, electrolyser assembly, membrane regulation, and electrolyte engineering. In addition, the challenges and future opportunities are highlighted for the development of seawater splitting technologies toward large-scale hydrogen production.

The majority of cellular physiological processes depend on natural ion channels, which are pore-forming membrane-embedded proteins that let ions flow across the cell membranes selectively. This selective movement of ions across the membranes balances the osmolality within and outside the cell. However, mutations in the genes that encode essential membrane transport proteins or structural reorganisation of these proteins can cause life-threatening diseases like cystic fibrosis. Artificial ion transport systems have opened up a way to replace dysfunctional natural ion channels to cure such diseases through channel replacement therapy. Moreover, recent research has also demonstrated the ability of these systems to kill cancer cells, reigniting interest in the field among scientists. Our contributions to the recent progress in the design and development of artificial chloride ion transporters and their effect on biological systems have been discussed in this review. This review would provide current vistas and future directions toward the development of novel ion transporters with…

Metal materials are susceptible to the influence of environmental media, and chemical or electrochemical multiphase reactions occur on the metal surface, resulting in the corrosion of metal materials, which can directly damage the geometry and reduce the physical properties of metal materials. This corrosion damage can seriously affect the long-term use of metal materials in marine equipment and the aerospace industry, and other fields. Inspired by the special microstructure and slippery properties of natural nepenthes intine, researchers have prepared slippery liquid-infused porous surfaces (SLIPS) with a stable continuous lubricant layer by injecting low-surface-energy lubricants into a substrate with a micro/nano-porous structure. This surface has excellent hydrophobicity, low friction, non-adhesiveness, and self-healing properties. The broad application prospects of SLIPS in the fields of anti-corrosion, anti-icing, anti-bacteria, and anti-fouling have made it a hot research topic directing the study of biomimetic materials at present. However, SLIPS are susceptible to…

The charge density of Co atoms in Co-MOFs is optimized by bimetallic (Fe, Ni) atom substitution, and the reconstructed Co(Ni)OOH on FeNiCo-MOF as the real active site lowers the energy barrier of rate-determining step, conducive to OER processes.

Functionalized bicyclo[2.1.1]hexanones are easily accessible via enolate addition to bicyclobutanes, including derivatives with an exocyclic amino group for further functionalization.

With the advent of a new era of smart-technology, the demand for more economic optoelectronic materials that do not compromise with efficiency is gradually on the rise. Organic semiconductors provide greener alternatives to the conventional inorganic ones, but encounter the challenge of balancing charge carrier mobility with processability in devices. Discotic liquid crystals (DLCs), a class of self-assembling soft organic materials, possess the perfect degree of order and dynamics to address this challenge. Providing unidimensional charge carrier pathways through their nanoscale columnar architecture, DLCs can behave as efficient charge transport systems across a wide range of optoelectronic devices. Moreover, DLCs are solution-processable, thus reducing the fabrication cost. In this article, we have discussed the approaches towards developing DLCs as semiconductors, focusing on their molecular design concepts, supramolecular structures and electronic properties in the context of their charge carrier mobilities.

stability at high temperatures) and tunability - doping both A- and B-site cations opens the path to a materials design approach that allows specific properties to be finely tuned towards applications. A major asset of perovskites is the ability to form nanoparticles on the surface under certain conditions in a process called "exsolution". Exsolution leads to the decoration of the material's surface with finely dispersed nanoparticles (which can be metallic or oxidic - depending on the experimental conditions) made from B-site cations of the perovskite lattice (here, doping comes into play, as B-site doping allows control over the constitution of the nanoparticles). In fact, the ability to undergo exsolution is one of the main reasons that perovskites are currently a hot topic of intensive research in catalysis and related fields. Exsolution on perovskites has been heavily researched in the last couple of years: various potential catalysts have been tested with different reactions, the oxide backbone materials and the exsolved nanoparticles have been investigated with a multitude of…

reduction. The important role of the doping state on affecting the photo-absorption, carrier separation efficiency, and photoreaction kinetics has been systemically investigated and proposed. This work sheds light on the future design and fabrication of high-performance photocatalysts by element doping.

non-covalent interactions and/or improved properties of existing materials. As a proof of concept, the crystal engineering approach to tackle two contemporary emergencies, namely, urea fertilizer degradation and development of antimicrobial resistance by pathogens, is discussed and application-driven examples are provided.

ZIF nanozyme with excellent peroxidase (POD)-like activity. The developed colorimetric sensor exhibits assay performance and offers a universal and promising analysis strategy for detecting OPs in practical samples.

Electroactive organic materials have received much attention as alternative electrodes for metal-ion batteries due to their high theoretical capacity, resource availability, and environmental friendliness. In particular, redox-active covalent organic frameworks (COFs) have recently emerged as promising electrodes due to their tunable electrochemical properties, insolubility in electrolytes, and structural versatility. In this Highlight, we review some recent strategies to improve the energy density and power density of COF electrodes for lithium batteries from the perspective of molecular design and electrode optimisation. Some other aspects such as stability and scalability are also discussed. Finally, the main challenges to improve their performance and future prospects for COF-based organic batteries are highlighted.

, the role of the amphiphile as a ligand obviating phosphine ligands in catalysis, the shielding effect of micelles to protect water-sensitive reaction intermediates in catalysis, and the compartmentalization effect. While compiling the powerful impact of micellar catalysis, this article highlights two diverse recent technologies: (i) the design and employment of the surfactant PS-750-M in selective catalysis; (ii) the use of the semisynthetic HPMC polymer to enable ultrafast reactions in water.

Carbon nanomaterials have enormous applications in various fields, such as adsorption, membrane separation, catalysis, electronics, capacitors, batteries, and medical sciences. Owing to their exceptional properties, such as large specific surface area, carrier mobility, flexibility, electrical conductivity, and optical pellucidity, the family of carbon nanomaterials is considered as one of the most studied group of materials to date. They are abundantly used in membrane science for multiple applications, such as the separation of organics, enantiomeric separation, gas separation, biomolecule separation, heavy metal separation, and wastewater treatment. This study provides an overview of the significant studies on carbon nanomaterial-based membranes and their emerging applications in our membrane research journey. The types of carbon nanomaterials, their utilization in membrane-based separations, and the mechanism involved are summarized in this study. Techniques for the fabrication of different nanocomposite membranes are also highlighted. Lastly, we have provided an overview of the…

, 1.59 V) and can remain stable for more than 100 h. Moreover, the theoretical calculations showed that CMPS features a suitable H* adsorption beneficial for the HER, as well as a lower free energy barrier favorable for the OER.

Molecular spectral signals can be significantly altered by solvent effects. Among the many theoretical approaches to this problem, continuum and atomistic solvation models have emerged as the most effective for properly describing solvent effects on the spectroscopic signal. In this feature article, we review the continuum and atomistic descriptions as applied to the calculation of molecular spectra, by detailing the similarities and differences between the two approaches from the formal point of view and by analyzing their advantages and disadvantages from the computational point of view. Various spectral signals, of increasing complexity, are considered and illustrative examples, selected to exacerbate the differences between the two approaches, are discussed.

Enantiomerically enriched sulfones occupy a prominent position in pharmaceutical chemistry and synthetic chemistry. Compared with conventional methods, a direct asymmetric sulfonylation reaction with the fixation of sulfur dioxide represents an attractive strategy for the rapid assembly of chiral sulfones with enantiopurity. In this highlight, we survey recent exciting advances in asymmetric sulfonylation by using sulfur dioxide surrogates, and discuss asymmetric induction modes, reaction mechanisms, substrate scope and opportunities for further studies.

Rhodamine-based chemosensors are widely used for the detection of various metal ions and applied in many fields of science including biological and environmental sciences. Rhodamine derivatives remain colorless and almost nonfluorescent when their spirolactam ring remains in closed form. They become pink or purple and strongly fluorescent upon opening of the ring. A particular metal ion can induce the ring opening process under a set of conditions and the process of selective sensing is dependent on many factors. Differentiation of metal sensing using rhodamine dyes is achieved in various ways which include selection of solvent, pH, mode of interaction with the cations, and so on. We have incorporated more than 140 research articles here to discuss the structure-property correlation of rhodamine based chemosensors. We have tried to correlate metal ion selectivity and structures of the chemosensors for the first time for rhodamine derivatives.

Metal complexes have shown promise as photosensitizers for cancer diagnosis and therapeutics. However, the vast majority of metal photosensitizers are not ideal and associated with several limitations including pharmacokinetic limitations, off-target toxicity, fast systemic clearance, poor membrane permeability, and hypoxic tumour microenvironments. Metal complex functionalized nanomaterials have the potential to construct multifunctional systems, which not only overcome the above defects of metal complexes but are also conducive to modulating the tumour microenvironment (TME) and employing combination therapies to boost photodynamic therapy (PDT) efficacy. In this review, we first introduce the current challenges of photodynamic therapy and summarize the recent research strategies (such as metal coordination bonds, self-assembly, π-π stacking, physisorption, and so on) used for preparing metal complexes functionalized nanomaterials in the application of PDT.

)-H bonds is a key chemical reaction in the production of fine chemicals and pharmaceuticals. Hydrogen atom transfer has recently gained significant attention for its ability to functionalise C-H bonds. The C-H bond can be activated by transferring the H radical to a hydrogen acceptor such as the chlorine radical (Cl˙). Thus, the Cl˙ generated by light irradiation can be used to initiate C-H oxygenation reactions, in which molecular oxygen is used as the oxidant. In this review article, we have summarised the recent advances in the field of Cl˙-mediated C-H oxygenation reactions. Reactions with catalysts such as metal chlorides, organophotoredox catalysts (acridinium ions), and chlorine dioxide radicals under light irradiation have been discussed. We conclude the review by providing suggestions for future research studies in the field. We expect that this review article will provide valuable information for the development of Cl˙-mediated C-H oxygenation reactions, contribute to the understanding of the reactivity of Cl˙, and inspire other useful synthetic chemical applications for…

Are lead-free perovskite-inspired materials (PIMs) the wise choice for efficient yet sustainable indoor light harvesting? This feature article outlines how wide-bandgap PIMs can provide a positive answer to this compelling question. The wide band gaps can hinder sunlight absorption, in turn limiting the solar cell performance. However, PIMs based on group VA of the periodic table can theoretically lead to an outstanding indoor power conversion efficiency up to 60% when their band gap is ∼2 eV. Yet, the research on PIM-based indoor photovoltaics (IPVs) is still in an early stage with highest indoor device efficiencies up to 10%. This article reviews the recent advancements on PIMs for IPVs and identifies the main limiting factors of device performance, thus suggesting effective strategies to address them. We emphasize the poor operational stability of the IPV devices of PIMs being the key bottleneck for the vast adoption of this technology. We believe that this report can provide a solid scaffolding for further researching this fascinating class of materials, ultimately supporting…

The effective capture of radioiodine is vital to the development of the nuclear industry and ecological environmental protection. There is, therefore, a continuously growing research exploration in various types of solid-state materials for iodine capture. During the last decade, the potential of using macrocycle and cage-based supramolecular materials in effective uptake and separation of radioactive iodine has been demonstrated. Interest in the application of these materials in iodine capture originates from their diversified porous characteristics, abundant host-guest chemistry, high iodine affinity and adsorption capacity, high stability in various environments, facile modification and functionalization, and intrinsic structural flexibility, among other attributes. Herein, recent progress in macrocycle and cage-based solid-state materials, including pure discrete macrocycles and cages, and their polymeric forms, for iodine capture is summarized and discussed with an emphasis on iodine capture capacities, mechanisms, and design strategies.

experiments, achieving strong NIR-II fluorescence tracing of tumors and impressive NIR-II image-guided photodynamic therapy (PDT) and photothermal therapy (PTT).

In this feature article, we aim at summarizing the design strategies of COF-based electrode materials for SCs based on the representative advances. The current challenges and future perspectives of COFs for SC application are highlighted as well.

An interface coupling strategy is developed to deposit metal W species onto Co 2 P nanosheets on a nickel foam substrate (W@Co 2 P/NF). This catalyst realizes superior bifunctional performance for both the HER and HzOR in an alkaline medium.

, sodium ion batteries, lithium-sulfur batteries, structural batteries, and hybrid supercapacitors. In this feature article, we provide a comprehensive overview of the strategies developed in our research to create graphene-based composite electrodes with better ionic conductivity, electron mobility, specific surface area, mechanical properties, and device performance than state-of-the-art electrodes. We summarize the strategies of structure manipulation and surface modification with specific focus on tackling the existing challenges in electrodes for batteries and supercapacitors by exploiting the unique properties of graphene-related materials.

ligands - a templating anion or borohydride" as an inexhaustible platform for the creation of new atomically precise clusters, superatoms, and nanoalloys.

The use of engineered ketoreductases (KREDS), both as whole microbial cells and isolated enzymes, in the highly enantiospecific reduction of prochiral ketones is reviewed. The homochiral alcohol products are key intermediates in, for example, pharmaceuticals synthesis. The application of sophisticated protein engineering and enzyme immobilisation techniques to increase industrial viability are discussed.

regulating surface wettability, designing pore structures and reducing crude oil viscosity. Meanwhile, the separation mechanisms, construction ideas, fabrication strategies, separation performances, practical applications, and the advantages and disadvantages of special wettable adsorption separation materials are also analyzed. Finally, the challenges and future prospects for adsorption separation of high-viscosity crude oil/water mixtures are expounded.

C -Glycoside analogs of naturally occurring glycoconjugates are useful tools for chemical biology studies, but their synthesis usually requires protection of the hydroxyl groups of the glycosyl donors.

conformers, leading to intriguing possibilities for chiral induction and sensing. By the introduction of bulky substituents on the rims, employing rotaxanation or pseudocatenation, planar chirality could be locked, enabling the enantiomeric separation of the chiral structures. The induced or separated chiral conformers/compounds exhibit significant chiroptical properties. These macrocyclic arenes, with flipping-induced inversion of planar chirality, demonstrated intriguing chiral induction dynamics and kinetics. In this featured review, we systematically summarize the progress in chiroptical induction/regulation of these macrocyclic arenes, particularly in the fields of chiral sensing, molecular machines, molecular recognition, and assembly.

Interfacial polymerization is a well-known process to synthesize separation layers for thin film composite membranes at an immiscible organic liquid-aqueous liquid interface. The organic-aqueous interface determines the diffusion dynamics of monomers and the chemical environment for polymerization, exerting a critical influence on the formation of polymer thin films. This review summarizes recent advances in tailoring interfacial polymerization using interfaces beyond the conventional alkane-water interface to achieve high-performance separation films with designed structures. Diverse liquid-liquid interfaces are introduced for synthesizing separation films by adding co-solvents into the organic phase and/or the aqueous phase, respectively, or by replacing one of the liquid phases with other solvents. Innovative liquid-gel and liquid-gas interfaces are then summarized for the synthesis of polymer thin films for separation. Novel strategies to form reaction interfaces, such as spray-coating, are also presented and discussed. In addition, we discuss the details of how a physically or…

Incorporation of Ir cations into Co 3 O 4 could cause a lattice expansion effect and thus promote both the hydrogen evolution reaction and the glycerol oxidation reaction.

An ultrasonic-assisted hydrothermal method is proven to reduce the size of RhCu nanospheres and improves the electrocatalytic performance for urea synthesis with a high faradaic efficiency of 34.82% and a high urea yield rate of 26.81 mmol g −1 h −1 .

M-NC catalysts were prepared by a combination of the electrospinning method and thermal treatment. For the first time, the contribution of N-species to the ORR (oxygen reduction reaction) of the M-NC was analysed using XPS (X-ray photoelectron spectroscopy). The obtained relations were verified by VASP (Vienna Ab-initio Simulation Package).

A LiF-involved molten-salt etching method is proposed for yielding delaminatable MXenes with comparable quality and supercapacitive performance to those made by solution etching. This approach combines the benefits of molten-salt etching in processability with high exfoliation efficiency of solution-based etching method.

Since the first introduction of their concept in the 1980s and 90s, polymer brushes have been the focus of intense research efforts to identify novel physico-chemical properties and responsiveness, and optimise the properties of associated interfaces for an ever growing range of applications. To a large extent, this effort has been enabled by progress in surface initiated controlled polymerisation techniques, allowing a huge diversity of monomers and macromolecular architectures to be harnessed and achieved. However, polymer functionalisation through chemical coupling of various moieties and molecular structures has also played an important role in expanding the molecular design toolbox of the field of polymer brush science. This perspective article reviews recent progress in polymer brush functionalisation, discussing a broad range of strategies for the side chain and end chain chemical modification of these polymer coatings. The impact of the brush architecture on associated coupling is also examined. In turn, the role that such functionalisation approaches play in the patterning…

Recent progress on catalytic nitrene transfer reactions with hydroxylamine derivatives as prevalent precursors is summarized in this highlight. The salient features of these N-O derived nitrene transfer reagents are that they are readily available, bench-stable, and can be facilely activated by a range of transition metal-catalysts under mild conditions. The application of these reagents in transition metal-catalysis has led to many new amidation or amination reactions, such as C-H insertions and aziridination of olefins. These reagents have also been applied in difunctionalisation of unsaturated bonds, dearomative amination of indoles, and formation of N-X bonds. Moreover, the recent achievements in photocatalysis and enzyme catalysis further emphasize the importance of these appealing reagents. This highlight provides an overview of these reactions reported in recent years. Challenges and potential opportunities for future developments are also discussed.

imaging applications. Taking advantage of the excellect penetration depth of acoustic signals, ultrasonic imaging has been widely applied for determining the location, size and shape of organs, identifying normal and abnormal tissues, as well as confirming the edges of lesions in hospitals. Thus, in the second section, we will briefly summarize recent advances in ultrasonic imaging techniques for diagnosing diseases in deep tissues. Nevertheless, the absence of lesion targeting and dependency on a professional technician may lead to the possibility of false-positive diagnosis. By combining the merits of both optical and acoustic signals, newly-developed photoacoustic imaging, simultaneously featuring higher temporal and spatial resolution with good sensitivity, as well as deeper penetration depth, is discussed in the third secretion. In the final part, we further discuss the major challenges and prospects for developing imaging technology for accurate disease diagnosis. We believe that these non-invasive imaging technologies will introduce a new perspective for the precise diagnosis…

Three-dimensional graphene (3DG)/metal-organic framework (MOF)-based composites have attracted more and more attention in the field of energy due to their unique hierarchical porous structure and properties. The combination of graphene with MOFs can not only effectively overcome the limitations of poor electrical conductivity and low stability of MOFs, but also prevent the aggregation and reaccumulation between graphene sheets. Moreover, 3DG/MOF composites can also be used as multifunctional precursors with adjustable structures and composition of derivatives, thus expanding their applications in the field of electrochemistry. This feature article elaborates the latest synthesis methods of 3DG/MOF composites and their derivatives, along with their applications in batteries, supercapacitors (SCs) and electrocatalysis. In addition, the current challenges and future prospects of 3DG/MOF-based composites are discussed.

doping with a low content of Y can tailor the electronic structure of the MOF structures, thereby improving their electrocatalytic performance for both hydrogen evolution and glycerol oxidation reactions.

The direct functionalization of alkanes represents a very important challenge in the goal to develop more atom-efficient and clean C-C bond forming reactions. These processes, however, are hampered by the low reactivity of the aliphatic C-H bonds. Photocatalytic processes based on hydrogen atom transfer C-H bond activation strategies have become a useful tool to activate and functionalize these inert compounds. In this article, we summarize the main achievements in this field applied to the development of C-C bond forming reactions, and we discuss the key mechanistic features that enable these transformations.

Chemical labeling of proteins in live cells helps to probe their native functions in biological systems. Aryl azides are chemically inert under physiological conditions, but they are activated by certain external stimuli. Recently, photocatalytic live-cell applications of aryl azides by visible light irradiation have become a burgeoning new field in chemical biology. In this Feature Article, we focus on the recent progress of protein labeling in live cells with aryl azides induced by visible-light irradiation. Light irradiation activates aryl azides to generate highly reactive intermediates, which enables protein labeling for protein functionalization, crosslinking, and profiling. The activation mechanism of aryl azides by light irradiation is categorized as photolysis, energy-transfer, and electron-transfer. The extracellular and intracellular protein labeling applications in live cells with aryl azides induced by visible light are discussed, including recent advances in red-light-induced extracellular protein labeling.

The reactions of enaminones, hydrazine hydrochlorides and internal alkynes for the synthesis of N -naphthyl pyrazoles are achieved via Rh( iii ) catalysis, representing the first three-component Satoh–Miura benzannulation.

A new Cu porphyrin bearing meso -( o -carborane) substituents is designed and synthesized and displays much higher activity than o -carborane-free analogues for the electrocatalytic hydrogen evolution reaction in both organic and aqueous solutions.