Chemical Society Reviews最新文献

{"title":"Rapid synthesis of metastable materials for electrocatalysis","authors":"Qiao Chen, Zichao Xi, Ziyuan Xu, Minghui Ning, Huimin Yu, Yuanmiao Sun, Da-Wei Wang, Ali Sami Alnaser, Huanyu Jin, Hui-Ming Cheng","doi":"10.1039/d5cs00090d","DOIUrl":"https://doi.org/10.1039/d5cs00090d","url":null,"abstract":"Metastable materials are considered promising electrocatalysts for clean energy conversions by virtue of their structural flexibility and tunable electronic properties. However, the exploration and synthesis of metastable electrocatalysts <em>via</em> traditional equilibrium methods face challenges because of the requirements of high energy and precise structural control. In this regard, the rapid synthesis method (RSM), with high energy efficiency and ultra-fast heating/cooling rates, enables the production of metastable materials under non-equilibrium conditions. However, the relationship between RSM and the properties of metastable electrocatalysts remains largely unexplored. In this review, we systematically examine the unique benefits of various RSM techniques and the mechanisms governing the formation of metastable materials. Based on these insights, we establish a framework, linking RSM with the electrocatalytic performance of metastable materials. Finally, we outline the future directions of this emerging field and highlight the importance of high-throughput approaches for the autonomous screening and synthesis of optimal electrocatalysts. This review aims to provide an in-depth understanding of metastable electrocatalysts, opening up new avenues for both fundamental research and practical applications in electrocatalysis.","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":"88 1","pages":""},"PeriodicalIF":46.2,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143744812","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Polysulfide chemistry in metal–sulfur batteries","authors":"Xi-Yao Li, Meng Zhao, Yun-Wei Song, Chen-Xi Bi, Zheng Li, Zi-Xian Chen, Xue-Qiang Zhang, Bo-Quan Li, Jia-Qi Huang","doi":"10.1039/d4cs00318g","DOIUrl":"https://doi.org/10.1039/d4cs00318g","url":null,"abstract":"Renowned for their high theoretical energy density and cost-effectiveness, metal–sulfur (M–S) batteries are pivotal in overcoming the current energy storage bottlenecks and accelerating the transition toward a cleaner society. Polysulfides (PSs) serve as essential intermediates in M–S batteries and bridge the electrochemical redox processes of sulfur, playing a decisive role in controlling the electrode behaviors and regulating the battery performances. Understanding PS chemistry across diverse battery environments is key to advancing M–S batteries. This review aims to provide a comprehensive overview of the PS chemistry in high-energy-density battery systems and outline future research directions. The compositions, properties, and characterization methods of PSs are introduced to facilitate a fundamental understanding of the PS chemistry in working batteries. Following this, a thorough examination of the chemical and electrochemical behaviors of PSs and their impacts on electrode performances is conducted to deepen the insights into the PS reactions in batteries. Building on this foundation, representative PS regulation strategies are discussed, focusing on molecular modification, solvation optimization, and interfacial regulation, to achieve superior M–S battery performances. Challenges of PSs in practical M–S batteries are finally analyzed, and perspectives on the future research trends of PS chemistry are presented.","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":"16 1","pages":""},"PeriodicalIF":46.2,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143744809","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Flexible iontronic sensing","authors":"Yang Li, Ningning Bai, Yu Chang, Zhiguang Liu, Jianwen Liu, Xiaoqin Li, Wenhao Yang, Hongsen Niu, Weidong Wang, Liu Wang, Wenhao Zhu, Di Chen, Tingrui Pan, Chuan Fei Guo, Guozhen Shen","doi":"10.1039/d4cs00870g","DOIUrl":"https://doi.org/10.1039/d4cs00870g","url":null,"abstract":"The emerging flexible iontronic sensing (FITS) technology has introduced a novel modality for tactile perception, mimicking the topological structure of human skin while providing a viable strategy for seamless integration with biological systems. With research progress, FITS has evolved from focusing on performance optimization and structural enhancement to a new phase of integration and intelligence, positioning it as a promising candidate for next-generation wearable devices. Therefore, a review from the perspective of technological development trends is essential to fully understand the current state and future potential of FITS devices. In this review, we examine the latest advancements in FITS. We begin by examining the sensing mechanisms of FITS, summarizing research progress in material selection, structural design, and the fabrication of active and electrode layers, while also analysing the challenges and bottlenecks faced by different segments in this field. Next, integrated systems based on FITS devices are reviewed, highlighting their applications in human–machine interaction, healthcare, and environmental monitoring. Additionally, the integration of artificial intelligence into FITS is explored, focusing on optimizing front-end device design and improving the processing and utilization of back-end data. Finally, building on existing research, future challenges for FITS devices are identified and potential solutions are proposed.","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":"39 1","pages":""},"PeriodicalIF":46.2,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143744811","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Gains and losses in zinc-ion batteries by proton- and water-assisted reactions","authors":"Yauhen Aniskevich, Seung-Taek Myung","doi":"10.1039/d4cs00810c","DOIUrl":"https://doi.org/10.1039/d4cs00810c","url":null,"abstract":"Research on aqueous zinc-ion batteries (AZIBs) has expanded significantly over the last decade due to their promising performance, cost, and safety as well as environmentally friendly features. The use of aqueous electrolytes enables promising AZIB properties while simultaneously introducing undesired reactions and processes. This review focuses on fundamental and critical considerations of water-related equilibria and reactions in zinc-ion batteries. First, we examine Zn<small>²⁺</small>/water ionic equilibria and their consequences for the chemistry of electrodes. Then, we focus on the mechanisms and kinetics of proton and Zn<small>²⁺</small> insertion in host frameworks. Next, special attention is given to the water-related dissolution, deposition, and amorphization phenomena of transition-metal-based cathode materials. Finally, we highlight the role of water- and proton-assisted reactions through a systematic comparison of aqueous and nonaqueous zinc-ion batteries.","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":"289 1","pages":""},"PeriodicalIF":46.2,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143736662","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Algorithm in chemistry: molecular logic gate-based data protection","authors":"Yu Dong, Shiyu Feng, Weiguo Huang and Xiang Ma","doi":"10.1039/D4CS01104J","DOIUrl":"10.1039/D4CS01104J","url":null,"abstract":"<p >Data security is crucial for safeguarding the integrity, authenticity, and confidentiality of documents, currency, merchant labels, and other paper-based assets, which sequentially has a profound impact on personal privacy and even national security. High-security-level logic data protection paradigms are typically limited to software (digital circuits) and rarely applied to physical devices using stimuli-responsive materials (SRMs). The main reason is that most SRMs lack programmable and controllable switching behaviors. Traditional SRMs usually produce static, singular, and highly predictable signals in response to stimuli, restricting them to simple “BUFFER” or “INVERT” logic operations with a low security level. However, recent advancements in SRMs have collectively enabled dynamic, multidimensional, and less predictable output signals under external stimuli. This breakthrough paves the way for sophisticated encryption and anti-counterfeiting hardware based on SRMs with complicated logic operations and algorithms. This review focuses on SRM-based data protection, emphasizing the integration of intricate logic and algorithms in SRM-constructed hardware, rather than chemical or material structural evolutions. It also discusses current challenges and explores the future directions of the field—such as combining SRMs with artificial intelligence (AI). This review fills a gap in the existing literature and represents a pioneering step into the uncharted territory of SRM-based encryption and anti-counterfeiting technologies.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" 8","pages":" 3681-3735"},"PeriodicalIF":40.4,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143736668","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Protein-derived cofactors: chemical innovations expanding enzyme catalysis","authors":"Angelica Graciano, Aimin Liu","doi":"10.1039/d4cs00981a","DOIUrl":"https://doi.org/10.1039/d4cs00981a","url":null,"abstract":"Protein-derived cofactors, formed through posttranslational modification of a single amino acid or covalent crosslinking of amino acid side chains, represent a rapidly expanding class of catalytic moieties that redefine enzyme functionality. Once considered rare, these cofactors are recognized across all domains of life, with their repertoire growing from 17 to 38 types in two decades in our survey. Their biosynthesis proceeds <em>via</em> diverse pathways, including oxidation, metal-assisted rearrangements, and enzymatic modifications, yielding intricate motifs that underpin distinctive catalytic strategies. These cofactors span paramagnetic and non-radical states, including both mono-radical and crosslinked radical forms, sometimes accompanied by additional modifications. While their discovery has accelerated, mechanistic understanding lags, as conventional mutagenesis disrupts cofactor assembly. Emerging approaches, such as site-specific incorporation of non-canonical amino acids, now enable precise interrogation of cofactor biogenesis and function, offering a viable and increasingly rigorous means to gain mechanistic insights. Beyond redox chemistry and electron transfer, these cofactors confer enzymes with expanded functionalities. Recent studies have unveiled new paradigms, such as long-range remote catalysis and redox-regulated crosslinks as molecular switches. Advances in structural biology, mass spectrometry, and biophysical spectroscopy continue to elucidate their mechanisms. Moreover, synthetic biology and biomimetic chemistry are increasingly leveraging these natural designs to engineer enzyme-inspired catalysts. This review integrates recent advances in cofactor biogenesis, reactivity, metabolic regulation, and synthetic applications, highlighting the expanding chemical landscape and growing diversity of protein-derived cofactors and their far-reaching implications for enzymology, biocatalysis, and biotechnology.","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":"218 1","pages":""},"PeriodicalIF":46.2,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723349","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Organo-mediator enabled electrochemical transformations","authors":"Weimei Zeng, Yanwei Wang, Chengyi Peng, Youai Qiu","doi":"10.1039/d4cs01142b","DOIUrl":"https://doi.org/10.1039/d4cs01142b","url":null,"abstract":"Electrochemistry has emerged as a powerful means to facilitate redox transformations in modern chemical synthesis. This review focuses on organo-mediators that facilitate electrochemical reactions <em>via</em> outer-sphere electron transfer (ET) between active mediators and substrates, offering advantages over direct electrolysis due to their availability, ease of modification, and simple post-processing. They prevent overoxidation/reduction, enhance selectivity, and mitigate electrode passivation during the electrosynthesis. By modifying the structure of organo-mediators, those with tunable redox potentials enable electrosynthesis and avoid metal residues in the final products, making them promising for further application in synthetic chemistry, particularly in pharmacochemistry, where the maximum allowed level of the metal residue in synthetic samples is extremely strict. This review highlights the recent advancements in this rapidly growing area within the past two decades, including the electrochemical organo-mediated oxidation (EOMO) and electrochemical organo-mediated reduction (EOMR) events. The organo-mediator enabled electrochemical transformations are discussed according to the reaction type, which has been categorized into oxidation and reduction organic mediators.","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":"87 1","pages":""},"PeriodicalIF":46.2,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723350","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"A surface chemistry perspective on SERS: revisiting the basics to push the field forward.","authors":"Chiara Deriu, Laura Fabris","doi":"10.1039/d4cs01242a","DOIUrl":"10.1039/d4cs01242a","url":null,"abstract":"<p><p>Surfaces are well known to be complex entities that are extremely difficult to study, and any phenomenon that is related to them is consequently challenging to approach. Moving from the bulk to the nanoscale adds a further layer of complexity to the problem. Because SERS relies on surfaces at the nanoscale, a rigorous understanding of the chemical phenomena that concur in the observation of the SERS signal is still limited or disorganized at best. Specifically, the lack of understanding of the chemical properties of nanoparticle surfaces has direct consequences on the development of SERS-based devices, causing a widespread belief that SERS is an inherently unreliable and fundamentally irreproducible analytical technique. Herein, we discuss old and new literature from SERS and related fields to accompany the reader through a journey that explores the chemical nature and architecture of colloidal plasmonic nanoparticles as the most popular SERS-active surfaces. By examining the chemistry of the surface landscape of the most common SERS colloids and the thermodynamic equilibria that characterize it, we aim to paint a chemically realistic picture of what a SERS analyst deals with on a daily basis. Thus, our goal for this review is to provide a centralized compilation of key, state-of-the-art surface chemistry information that can guide the rational development of analytical protocols and contribute an additional path through which our community can continue to advance SERS as a reliable and robust analytical tool.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" ","pages":""},"PeriodicalIF":40.4,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11937889/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143707833","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"A review of Ni-based layered oxide cathode materials for alkali-ion batteries.","authors":"Lei Wang, Jiaqing Wang, Yifei Lu, Suqiao Fang, Chao Yang, Xingqiao Wu, Yao Xiao, Yong Wang, Shulei Chou, Shuangqiang Chen","doi":"10.1039/d3cs00911d","DOIUrl":"https://doi.org/10.1039/d3cs00911d","url":null,"abstract":"<p><p>Compared with the costly and toxic LiCoO₂ cathode in lithium-ion batteries (LIBs), nickel-based layered oxide (NLO) cathode materials exhibit the advantages of high capacity, natural abundance, environment-friendliness, and low cost, displaying tremendous application potentials in power batteries for automobiles and aircrafts. This review comprehensively introduces the challenges faced by NLO cathode materials in all alkali-ion batteries (AIBs) in their material synthesis, cation mixing, particle cracking, phase changes, cation dissolution of Mn, and oxygen loss Various strategies, including heteroatom doping, surface coating, and concentration gradient, are applied to tackle these problems by developing layered LiNi_1-<i>x</i>M_<i>x</i>O₂ (M: metal; 0 < <i>x</i> < 1) and LiNi_<i>x</i>Co_<i>y</i>Mn_<i>z</i>O₂ (<i>x</i> + <i>y</i> + <i>z</i> = 1) materials. The successful commercial application of NLO cathode materials in LIBs has further driven their developments in sodium/potassium-ion batteries <i>via</i> the synthesis of (Na/K)Ni_1-<i>x</i>M_<i>x</i>O₂. Moreover, many sophisticated techniques, including <i>in situ</i> X-ray diffraction, scanning/transmission electron microscopy, <i>operando</i> neutron diffraction, and elemental analysis, are used to simultaneously monitor real-time phase changes, lattice variations, structural distortions, and elemental dissolutions of NLO-based materials. Furthermore, density functional theory (DFT) calculations are discussed as a powerful tool for predicting structural evolution, energy band structures, optimal doping concentrations, and ion diffusion pathways, thereby guiding the reasonable design of these materials. Finally, this review provides perspectives on future research directions and modification strategies for NLO cathode materials in AIBs, aiming to accelerate their deployment in electric vehicles and other energy storage devices. These efforts are expected to contribute significantly to the advancement of sustainable energy technologies and the global pursuit for carbon neutrality.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" ","pages":""},"PeriodicalIF":40.4,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143707824","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Self-healing behavior of superhard covalent bond materials","authors":"Keliang Qiu, Xiang Li, Yanhong Li, Yonghai Yue, Lin Guo","doi":"10.1039/d4cs01182a","DOIUrl":"https://doi.org/10.1039/d4cs01182a","url":null,"abstract":"In recent years, superhard covalently bonded materials have drawn a great deal of attention due to their excellent mechanical properties and potential applications in various fields. This review focuses on the self-healing behavior of these materials, outlining state-of-the-art research results. In detail, we discuss current self-healing mechanisms of self-healing materials including extrinsic healing mechanisms (such as microencapsulation, oxidative healing, shape memory, <em>etc.</em>) and intrinsic healing (dynamic covalent bonding, supramolecular interactions, diffusion, defect-driven processes, <em>etc.</em>). We also provide an overview of the progress in the self-healing behavior of superhard covalently bonded materials and the mechanisms of permanent covalent bonding healing. Additionally, we analyze the factors that influence the healing properties of these materials. Finally, the main findings and an outlook on the future directions and challenges of this emerging field are summarized in the Conclusion section.","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":"123 1","pages":""},"PeriodicalIF":46.2,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143677602","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}