Li Wang, Yide Jiao, Hongjie Zhang, Yaqing Liu, Yujia Zhang, Peiyi Wu, Kai Xiao
The human brain efficiently processes external information using ions as information carriers, inspiring the development of ionic brain-like intelligence. Central to such systems are neuromorphic iontronic devices (NIDs), including artificial axons, synapses, and neurons, which employ ions as charge carriers. Recently, NIDs based on soft ionic conductors (SICs), such as ionic hydrogels, ionogels, and ionic elastomers, have attracted growing attention due to their ionic compatibility, flexibility, biocompatibility, and facile fabrication and integration, making them promising candidates for next-generation neuromorphic technologies. Despite their potential, research remains in its infancy, with key challenges in elucidating fundamental mechanisms, establishing design principles, and realizing practical applications. To address these issues and guide future research, this review first introduces the functional roles and electrical signalling of axons, synapses, and neurons, thereby defining the performance requirements for NIDs. It then summarizes means for controlling ion transport in SICs and discusses feasible approaches for constructing SIC-based NIDs, including structural and interfacial engineering, device architectures, and dropletronic techniques. Finally, recent advances in SIC-based NIDs are reviewed, and their prospects in human–machine interaction and brain-like computing are discussed along with the remaining challenges.
{"title":"Neuromorphic iontronic devices based on soft ionic conductors","authors":"Li Wang, Yide Jiao, Hongjie Zhang, Yaqing Liu, Yujia Zhang, Peiyi Wu, Kai Xiao","doi":"10.1039/d5cs00580a","DOIUrl":"https://doi.org/10.1039/d5cs00580a","url":null,"abstract":"The human brain efficiently processes external information using ions as information carriers, inspiring the development of ionic brain-like intelligence. Central to such systems are neuromorphic iontronic devices (NIDs), including artificial axons, synapses, and neurons, which employ ions as charge carriers. Recently, NIDs based on soft ionic conductors (SICs), such as ionic hydrogels, ionogels, and ionic elastomers, have attracted growing attention due to their ionic compatibility, flexibility, biocompatibility, and facile fabrication and integration, making them promising candidates for next-generation neuromorphic technologies. Despite their potential, research remains in its infancy, with key challenges in elucidating fundamental mechanisms, establishing design principles, and realizing practical applications. To address these issues and guide future research, this review first introduces the functional roles and electrical signalling of axons, synapses, and neurons, thereby defining the performance requirements for NIDs. It then summarizes means for controlling ion transport in SICs and discusses feasible approaches for constructing SIC-based NIDs, including structural and interfacial engineering, device architectures, and dropletronic techniques. Finally, recent advances in SIC-based NIDs are reviewed, and their prospects in human–machine interaction and brain-like computing are discussed along with the remaining challenges.","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":"3 1","pages":""},"PeriodicalIF":46.2,"publicationDate":"2025-12-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145658045","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}
Correction for 'Organoantimony: a versatile main-group platform for pnictogen-bonding and redox catalysis' by Elisa Chakraborty et al., Chem. Soc. Rev., 2025, https://doi.org/10.1039/d3cs00332a.
{"title":"Correction: Organoantimony: a versatile main-group platform for pnictogen-bonding and redox catalysis.","authors":"Elisa Chakraborty, Robin Weiss","doi":"10.1039/d5cs90104a","DOIUrl":"10.1039/d5cs90104a","url":null,"abstract":"<p><p>Correction for 'Organoantimony: a versatile main-group platform for pnictogen-bonding and redox catalysis' by Elisa Chakraborty <i>et al.</i>, <i>Chem. Soc. Rev.</i>, 2025, https://doi.org/10.1039/d3cs00332a.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" ","pages":""},"PeriodicalIF":39.0,"publicationDate":"2025-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145653154","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}
Adhesive hydrogels represent a transformative technology in biomedicine due to their biocompatibility and multifunctionality. While extensive research has focused on improving their adhesion strength, the pursuit of long-term interfacial stability reveals a core conflict: strong adhesion often comes at the expense of easy removal. Dynamically regulating hydrogel adhesion is thus key to personalized medicine, allowing adaptation to complex clinical needs. Designing such systems demands a multifaceted approach that considers the physiological environment, medical requirements, stimulus-induced interfacial rearrangements, and mechanics-driven microstructure reconstruction. The dynamic regulation of hydrogel adhesion is more than a functional upgrade; it represents a paradigm shift for smart materials, from “static design” to “dynamic interaction”. This review first introduces the mechanisms of hydrogel adhesion. It then provides an in-depth analysis of strategies for dynamically regulating adhesion at the tissue–hydrogel interface and explores the latest progress and application potential in biomedicine.
{"title":"Dynamic regulation of interfacial adhesion in biomedical hydrogels","authors":"Hanjun Sun, Xinyu Qu, Qian Wang, Yuxin Guo, Xiaochen Dong","doi":"10.1039/d5cs00403a","DOIUrl":"https://doi.org/10.1039/d5cs00403a","url":null,"abstract":"Adhesive hydrogels represent a transformative technology in biomedicine due to their biocompatibility and multifunctionality. While extensive research has focused on improving their adhesion strength, the pursuit of long-term interfacial stability reveals a core conflict: strong adhesion often comes at the expense of easy removal. Dynamically regulating hydrogel adhesion is thus key to personalized medicine, allowing adaptation to complex clinical needs. Designing such systems demands a multifaceted approach that considers the physiological environment, medical requirements, stimulus-induced interfacial rearrangements, and mechanics-driven microstructure reconstruction. The dynamic regulation of hydrogel adhesion is more than a functional upgrade; it represents a paradigm shift for smart materials, from “static design” to “dynamic interaction”. This review first introduces the mechanisms of hydrogel adhesion. It then provides an in-depth analysis of strategies for dynamically regulating adhesion at the tissue–hydrogel interface and explores the latest progress and application potential in biomedicine.","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":"359 1","pages":""},"PeriodicalIF":46.2,"publicationDate":"2025-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145651017","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}
Tianpeng Huang, Yue Zheng, Deye Sun, Jun Ma, Pengxian Han, Guanglei Cui
Solid-state lithium metal batteries (SSLMBs) are considered ideal candidates for the next-generation core technologies for development of clean energy storage and conversion systems owing to their inherent high energy density and exceptional safety. Nevertheless, the practical energy density, power characteristics, and cycling stability of SSLMBs are usually limited by sluggish charge transfer kinetics within and across solid-state components, including electrode, electrolyte, binder, and conductive additive materials. Therefore, understanding the intrinsic link between structure–charge transport–performance and improving charge transport kinetics in a heterogeneous solid system through structural modulation has become the key to comprehensively improving the electrochemical performance of SSLMBs. Herein, a unique perspective is proposed to optimize the short-range and long-range charge transport processes in SSLMBs through multi-level structural modulation at the electrode, solid electrolyte, and cell levels. We firstly summarize and evaluate the research progress in multi-level structural modulation. Then, the vital factors impacting structural regulation and regulation principles at the corresponding level are analyzed in depth. Furthermore, the extent of enhancement and limitations of various structural modulation approaches employed for charge transport are evaluated and compared. At the end, perspectives and suggestions were provided on principles for multi-level structural modulation toward fast charge transport kinetics in inorganic SSLMBs. This review will offer broadly applicable principles for the development of next-generation high-performance inorganic SSLMBs.
{"title":"Multi-level structural modulation enables fast lithium-ion transport in inorganic solid-state batteries","authors":"Tianpeng Huang, Yue Zheng, Deye Sun, Jun Ma, Pengxian Han, Guanglei Cui","doi":"10.1039/d5cs00895f","DOIUrl":"https://doi.org/10.1039/d5cs00895f","url":null,"abstract":"Solid-state lithium metal batteries (SSLMBs) are considered ideal candidates for the next-generation core technologies for development of clean energy storage and conversion systems owing to their inherent high energy density and exceptional safety. Nevertheless, the practical energy density, power characteristics, and cycling stability of SSLMBs are usually limited by sluggish charge transfer kinetics within and across solid-state components, including electrode, electrolyte, binder, and conductive additive materials. Therefore, understanding the intrinsic link between structure–charge transport–performance and improving charge transport kinetics in a heterogeneous solid system through structural modulation has become the key to comprehensively improving the electrochemical performance of SSLMBs. Herein, a unique perspective is proposed to optimize the short-range and long-range charge transport processes in SSLMBs through multi-level structural modulation at the electrode, solid electrolyte, and cell levels. We firstly summarize and evaluate the research progress in multi-level structural modulation. Then, the vital factors impacting structural regulation and regulation principles at the corresponding level are analyzed in depth. Furthermore, the extent of enhancement and limitations of various structural modulation approaches employed for charge transport are evaluated and compared. At the end, perspectives and suggestions were provided on principles for multi-level structural modulation toward fast charge transport kinetics in inorganic SSLMBs. This review will offer broadly applicable principles for the development of next-generation high-performance inorganic SSLMBs.","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":"196 1","pages":""},"PeriodicalIF":46.2,"publicationDate":"2025-11-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145611744","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}
Jun Li, Yuling Xu, Yida Pang, Fang Zhao, Wenjun Zhang, Chonglu Li, Honglin Jin, Chao Yuan, Suhua Wang, Yao Sun
Precision medicine is aimed at achieving a more personalized approach tailored to individual characteristics and urgently requires the development of precise diagnostic and therapeutic methods. Small-molecule dyes play indispensable roles in medical imaging and surgery procedures, attracting significant attention regarding disease diagnosis and therapy. However, their widespread utilization for accurate tumor localization and long-term intraoperative imaging remains hindered by their inherent limitations, including tedious synthesis protocols, poor photostability, susceptibility to fluorescence quenching in physiological environments, and rapid systemic clearance. Supramolecular dyes, defined as small-molecule dye-based assemblies, usually present unique and superior photophysical properties, including tunable optical properties, enhanced photodynamic and photothermal performance, improved photostability and optimized anti-quenching capability, collectively enabling high-precision optical diagnosis and therapy. Despite remarkable progress in supramolecular dyes, a systemic review summarizing their applications in precision biomedicine remains lacking. In this review, we systematically summarize the recent advances on the development of supramolecular dyes across three key self-assembly systems: supramolecular coordination complexes (SCCs) systems, host–guest systems (including cyclodextrin, cucurbit[n]urils (CB [n]s), calixarenes and pillararenes), and enzyme instructed self-assembly (EISA) systems. Moreover, we highlight current challenges and future perspectives to accelerate their translation from fundamental research to clinical applications.
{"title":"Supramolecular dyes: advancing precision medicine through molecular engineering","authors":"Jun Li, Yuling Xu, Yida Pang, Fang Zhao, Wenjun Zhang, Chonglu Li, Honglin Jin, Chao Yuan, Suhua Wang, Yao Sun","doi":"10.1039/d5cs00734h","DOIUrl":"https://doi.org/10.1039/d5cs00734h","url":null,"abstract":"Precision medicine is aimed at achieving a more personalized approach tailored to individual characteristics and urgently requires the development of precise diagnostic and therapeutic methods. Small-molecule dyes play indispensable roles in medical imaging and surgery procedures, attracting significant attention regarding disease diagnosis and therapy. However, their widespread utilization for accurate tumor localization and long-term intraoperative imaging remains hindered by their inherent limitations, including tedious synthesis protocols, poor photostability, susceptibility to fluorescence quenching in physiological environments, and rapid systemic clearance. Supramolecular dyes, defined as small-molecule dye-based assemblies, usually present unique and superior photophysical properties, including tunable optical properties, enhanced photodynamic and photothermal performance, improved photostability and optimized anti-quenching capability, collectively enabling high-precision optical diagnosis and therapy. Despite remarkable progress in supramolecular dyes, a systemic review summarizing their applications in precision biomedicine remains lacking. In this review, we systematically summarize the recent advances on the development of supramolecular dyes across three key self-assembly systems: supramolecular coordination complexes (SCCs) systems, host–guest systems (including cyclodextrin, cucurbit[<em>n</em>]urils (CB [<em>n</em>]s), calixarenes and pillararenes), and enzyme instructed self-assembly (EISA) systems. Moreover, we highlight current challenges and future perspectives to accelerate their translation from fundamental research to clinical applications.","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":"109 1","pages":""},"PeriodicalIF":46.2,"publicationDate":"2025-11-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145611745","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}
The oxygen evolution reaction (OER) constitutes a critical half-reaction in electrochemical water splitting and plays a central role in sustainable energy conversion systems. This review commences with an overview of the fundamental principles governing the OER, serving as the conceptual basis for understanding the influence of external physical fields on catalytic behaviour. The individual effects of magnetic, photo, and thermal fields on OER kinetics and mechanisms are systematically examined, followed by an exploration of the coupling phenomena that arise from their concurrent application. Building on these mechanistic insights, we further discuss catalyst design strategies that exploit both isolated and synergistic external field effects, as reported in recent studies. Advances in computational screening and descriptor-guided design methodologies are also reviewed. Finally, we outline critical future directions, including the optimization of performance trade-offs among activity, stability, and energy efficiency, the development of standardized evaluation protocols, and the integration of theoretical modelling to guide rational catalyst development. Collectively, this review provides a comprehensive framework for advancing OER catalysis through the strategic application of external physical fields.
{"title":"Harnessing magnetic, photo, and thermal fields and their synergistic interactions for enhanced electrocatalytic oxygen evolution reaction","authors":"Yuan Cao, Linfeng Gao, Yijiang Liu, Zhiqun Lin","doi":"10.1039/d5cs00574d","DOIUrl":"https://doi.org/10.1039/d5cs00574d","url":null,"abstract":"The oxygen evolution reaction (OER) constitutes a critical half-reaction in electrochemical water splitting and plays a central role in sustainable energy conversion systems. This review commences with an overview of the fundamental principles governing the OER, serving as the conceptual basis for understanding the influence of external physical fields on catalytic behaviour. The individual effects of magnetic, photo, and thermal fields on OER kinetics and mechanisms are systematically examined, followed by an exploration of the coupling phenomena that arise from their concurrent application. Building on these mechanistic insights, we further discuss catalyst design strategies that exploit both isolated and synergistic external field effects, as reported in recent studies. Advances in computational screening and descriptor-guided design methodologies are also reviewed. Finally, we outline critical future directions, including the optimization of performance trade-offs among activity, stability, and energy efficiency, the development of standardized evaluation protocols, and the integration of theoretical modelling to guide rational catalyst development. Collectively, this review provides a comprehensive framework for advancing OER catalysis through the strategic application of external physical fields.","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":"6 1","pages":""},"PeriodicalIF":46.2,"publicationDate":"2025-11-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145609064","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}
Jaeyong Ahn, Wonbin Choi, Sang Hyuk Lee, Jonghyun Park, Seoyoung Kim, Inho Song, Joon Hak Oh
Because circularly polarized light (CPL) uniquely carries spin-selective information, chiral optoelectronics offer a powerful platform for developing high-efficiency, spin-based optical devices and driving next-generation photonic technologies. Intrinsically chiral semiconductors can absorb or emit CPL through light–matter interactions, positioning them as highly attractive active materials for advanced optoelectronics. However, their weak chiroptical activities often hinder practical implementation. To address this challenge, researchers have explored a range of strategies aimed at enhancing chiroptical performance. Recent advances in molecular design, processing techniques, and device engineering have led to significant improvements in the chiroptical properties of these materials. This review summarizes recent progress in chirality amplification strategies for semiconductors in advanced optoelectronics. Intrinsically chiral semiconductors are classified into three groups: organic semiconductors, metal–organic materials, and chiral hybrid perovskites. Furthermore, strategies for enhancing chiroptical signal output in chiral optoelectronic devices are discussed, supported by relevant theoretical frameworks. These advancements establish a solid foundation for the development of high-performance chiral optoelectronic devices, paving the way for future innovations in photonic technology.
{"title":"Chirality amplification in semiconductors for advanced optoelectronics","authors":"Jaeyong Ahn, Wonbin Choi, Sang Hyuk Lee, Jonghyun Park, Seoyoung Kim, Inho Song, Joon Hak Oh","doi":"10.1039/d5cs00684h","DOIUrl":"https://doi.org/10.1039/d5cs00684h","url":null,"abstract":"Because circularly polarized light (CPL) uniquely carries spin-selective information, chiral optoelectronics offer a powerful platform for developing high-efficiency, spin-based optical devices and driving next-generation photonic technologies. Intrinsically chiral semiconductors can absorb or emit CPL through light–matter interactions, positioning them as highly attractive active materials for advanced optoelectronics. However, their weak chiroptical activities often hinder practical implementation. To address this challenge, researchers have explored a range of strategies aimed at enhancing chiroptical performance. Recent advances in molecular design, processing techniques, and device engineering have led to significant improvements in the chiroptical properties of these materials. This review summarizes recent progress in chirality amplification strategies for semiconductors in advanced optoelectronics. Intrinsically chiral semiconductors are classified into three groups: organic semiconductors, metal–organic materials, and chiral hybrid perovskites. Furthermore, strategies for enhancing chiroptical signal output in chiral optoelectronic devices are discussed, supported by relevant theoretical frameworks. These advancements establish a solid foundation for the development of high-performance chiral optoelectronic devices, paving the way for future innovations in photonic technology.","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":"19 1","pages":""},"PeriodicalIF":46.2,"publicationDate":"2025-11-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145599836","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}
Qing Wang, Zhifang Zhou, Chang Liu, Yunpeng Zheng, Zongmo Shi, Bin Wei, Wenyu Zhang, Ce-Wen Nan, Yuan-Hua Lin
Oxide thermoelectric materials have emerged as promising candidates for sustainable energy applications owing to their inherent thermal stability, environmental benignity, elemental abundance, and low cost. This review comprehensively summarizes the recent advances in oxide thermoelectrics, covering synthesis methodologies for bulk and thin-film oxides as well as state-of-the-art advances in thermoelectric performance. Particular emphasis is placed on multiple optimization strategies aimed at carrier-phonon decoupling in oxides (such as high entropy design, texturization, homo-structure construction, and symmetry modulation) and emerging applications based on oxide thermoelectrics (including the photothermoelectric effect, and transverse thermoelectric effect), distinguished from conventional thermoelectric energy conversion. These coupled functionalities open new avenues for multi-modal energy harvesting and intelligent device integration. Finally, we highlight critical challenges and unresolved issues that need to be addressed in future research and practical applications in oxide thermoelectrics.
{"title":"Advances in oxide thermoelectric materials: strategies, applications and beyond","authors":"Qing Wang, Zhifang Zhou, Chang Liu, Yunpeng Zheng, Zongmo Shi, Bin Wei, Wenyu Zhang, Ce-Wen Nan, Yuan-Hua Lin","doi":"10.1039/d5cs01078k","DOIUrl":"https://doi.org/10.1039/d5cs01078k","url":null,"abstract":"Oxide thermoelectric materials have emerged as promising candidates for sustainable energy applications owing to their inherent thermal stability, environmental benignity, elemental abundance, and low cost. This review comprehensively summarizes the recent advances in oxide thermoelectrics, covering synthesis methodologies for bulk and thin-film oxides as well as state-of-the-art advances in thermoelectric performance. Particular emphasis is placed on multiple optimization strategies aimed at carrier-phonon decoupling in oxides (such as high entropy design, texturization, homo-structure construction, and symmetry modulation) and emerging applications based on oxide thermoelectrics (including the photothermoelectric effect, and transverse thermoelectric effect), distinguished from conventional thermoelectric energy conversion. These coupled functionalities open new avenues for multi-modal energy harvesting and intelligent device integration. Finally, we highlight critical challenges and unresolved issues that need to be addressed in future research and practical applications in oxide thermoelectrics.","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":"2 1","pages":""},"PeriodicalIF":46.2,"publicationDate":"2025-11-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145599835","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}
Yaoxiao Zhao,Mengyang Li,Wangqiang Shen,Kun Guo,Lipiao Bao,Xing Lu
Carbon is an incredibly versatile element and can form bonds via sp, sp2, and sp3 hybridization, forming diverse structures, which are responsible for the vast complexity and diversity of chemistry and biology. Therefore, understanding carbon bonding is crucial for comprehending the fundamental principles of natural science. Beyond conventional chemistry, carbon bonding confined inside carbon cages can adopt unusual and seemingly unpredictable bond states. Within these spatially restricted environments, encapsulated carbon atoms can bond with multiple nonmetal atoms (e.g., H, C, N, and O) and a variety of metal atoms (e.g., Sc, V, Ti, and Dy), forming otherwise unstable clusters with different bonding models and oxidation states of carbon. This leads to unprecedented bonding situations, including multiple and multicenter carbon-metal bonds, covalent carbon-metal bonds, superatomic states, and pronounced donation bonds (e.g. C2 → metal atoms). These bonding situations enrich the carbon bonding models beyond traditional organic chemistry. This review provides a comprehensive summary of the recent findings regarding constrained carbon bonding with varying numbers of carbon atoms inside carbon cages. It will encompass crucial aspects of this special constrained carbon bonding such as the dispersion of negative charge on the carbon cage, reduction of Coulomb repulsion, maximization of coordinated metal ions, and determination of optimal configurations for metal atoms within the carbon cages. Accordingly, new carbon bonding could be identified in carbon cages, which holds significant implications in the development of innovative carbon-based compounds. Additionally, the current challenges faced and future developments anticipated from the aspect of confined carbon bonding inside carbon cages will be discussed to provide deeper insights into the intricacies of carbon bonding. Through this comprehensive exploration, we hope to advance knowledge in this exciting area of carbon chemistry.
{"title":"Constrained carbon bonding inside fullerene cages.","authors":"Yaoxiao Zhao,Mengyang Li,Wangqiang Shen,Kun Guo,Lipiao Bao,Xing Lu","doi":"10.1039/d5cs00481k","DOIUrl":"https://doi.org/10.1039/d5cs00481k","url":null,"abstract":"Carbon is an incredibly versatile element and can form bonds via sp, sp2, and sp3 hybridization, forming diverse structures, which are responsible for the vast complexity and diversity of chemistry and biology. Therefore, understanding carbon bonding is crucial for comprehending the fundamental principles of natural science. Beyond conventional chemistry, carbon bonding confined inside carbon cages can adopt unusual and seemingly unpredictable bond states. Within these spatially restricted environments, encapsulated carbon atoms can bond with multiple nonmetal atoms (e.g., H, C, N, and O) and a variety of metal atoms (e.g., Sc, V, Ti, and Dy), forming otherwise unstable clusters with different bonding models and oxidation states of carbon. This leads to unprecedented bonding situations, including multiple and multicenter carbon-metal bonds, covalent carbon-metal bonds, superatomic states, and pronounced donation bonds (e.g. C2 → metal atoms). These bonding situations enrich the carbon bonding models beyond traditional organic chemistry. This review provides a comprehensive summary of the recent findings regarding constrained carbon bonding with varying numbers of carbon atoms inside carbon cages. It will encompass crucial aspects of this special constrained carbon bonding such as the dispersion of negative charge on the carbon cage, reduction of Coulomb repulsion, maximization of coordinated metal ions, and determination of optimal configurations for metal atoms within the carbon cages. Accordingly, new carbon bonding could be identified in carbon cages, which holds significant implications in the development of innovative carbon-based compounds. Additionally, the current challenges faced and future developments anticipated from the aspect of confined carbon bonding inside carbon cages will be discussed to provide deeper insights into the intricacies of carbon bonding. Through this comprehensive exploration, we hope to advance knowledge in this exciting area of carbon chemistry.","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":"223 1","pages":""},"PeriodicalIF":46.2,"publicationDate":"2025-11-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145583400","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}
Kwing Yeung Chan, Chenjie Zhuang, Vinh Gia Vuong, Naixin Qian, Xin Gao, Wei Min
Water at interfaces exhibits unique properties that differ markedly from those of bulk water. In particular, a myriad of water-interface-related enhanced reactivities including on-water catalysis and microdroplet chemistry have been documented since the 1980s but remain mechanistically unclear. This review focuses on recent advances in optical spectroscopy and imaging techniques—including fluorescence imaging, vibrational Stark spectroscopy, electrochromism, sum-frequency generation, and high-resolution Raman micro-spectroscopy—that have successfully enabled the detection of interfacial electric fields at different hydrophobic water interfaces (air, liquid and solid). We summarize how both probe-based and label-free optical spectroscopic techniques can consistently quantify the on-water electric field strengths to be on the order of tens of MV cm−1, corroborated by independent non-spectroscopic techniques, such as electrokinetic and surface charge measurements. The surprisingly close agreement among these different measurements and across broad experimental systems strongly hints at the existence of strong electric fields being a general feature of water–hydrophobe interfaces. We further discuss the physical origins of the interfacial electric field with a particular emphasis on the mechanism of preferential hydroxide accumulation at hydrophobic interfaces. Finally, we examine the implications of strong interfacial electric fields for chemical kinetics, radical generation and thermodynamics, thereby making important connections to interfacial water reactivity. These insights not only contribute to our fundamental understanding of water at interfaces but also point toward new strategies for harnessing interfacial water electrostatics in biomedicine, catalysis, green chemistry, and environmental science.
界面处的水表现出与散装水明显不同的独特性质。特别是,自20世纪80年代以来,无数与水界面相关的增强反应性,包括水上催化和微滴化学,已被记录在案,但其机制仍不清楚。本文综述了光谱学和成像技术的最新进展,包括荧光成像、振动斯塔克光谱、电致变色、和频产生和高分辨率拉曼微光谱,这些技术已经成功地检测了不同疏水水界面(空气、液体和固体)的界面电场。我们总结了基于探针和无标签的光谱学技术如何能够一致地将水中电场强度量化到几十MV cm - 1的量级,并通过独立的非光谱学技术(如电动力学和表面电荷测量)加以证实。在这些不同的测量和广泛的实验系统之间惊人的紧密一致强烈暗示了强电场的存在是疏水界面的一般特征。我们进一步讨论了界面电场的物理起源,特别强调了氢氧化物在疏水界面上的优先积累机制。最后,我们研究了强界面电场对化学动力学、自由基生成和热力学的影响,从而建立了与界面水反应性的重要联系。这些见解不仅有助于我们对界面水的基本理解,而且还指出了在生物医学、催化、绿色化学和环境科学中利用界面水静电的新策略。
{"title":"Electric fields at hydrophobic water interfaces: spectroscopic evidence, physical origin, and implications on reactivity","authors":"Kwing Yeung Chan, Chenjie Zhuang, Vinh Gia Vuong, Naixin Qian, Xin Gao, Wei Min","doi":"10.1039/d5cs00778j","DOIUrl":"https://doi.org/10.1039/d5cs00778j","url":null,"abstract":"Water at interfaces exhibits unique properties that differ markedly from those of bulk water. In particular, a myriad of water-interface-related enhanced reactivities including on-water catalysis and microdroplet chemistry have been documented since the 1980s but remain mechanistically unclear. This review focuses on recent advances in optical spectroscopy and imaging techniques—including fluorescence imaging, vibrational Stark spectroscopy, electrochromism, sum-frequency generation, and high-resolution Raman micro-spectroscopy—that have successfully enabled the detection of interfacial electric fields at different hydrophobic water interfaces (air, liquid and solid). We summarize how both probe-based and label-free optical spectroscopic techniques can consistently quantify the on-water electric field strengths to be on the order of tens of MV cm<small><sup>−1</sup></small>, corroborated by independent non-spectroscopic techniques, such as electrokinetic and surface charge measurements. The surprisingly close agreement among these different measurements and across broad experimental systems strongly hints at the existence of strong electric fields being a general feature of water–hydrophobe interfaces. We further discuss the physical origins of the interfacial electric field with a particular emphasis on the mechanism of preferential hydroxide accumulation at hydrophobic interfaces. Finally, we examine the implications of strong interfacial electric fields for chemical kinetics, radical generation and thermodynamics, thereby making important connections to interfacial water reactivity. These insights not only contribute to our fundamental understanding of water at interfaces but also point toward new strategies for harnessing interfacial water electrostatics in biomedicine, catalysis, green chemistry, and environmental science.","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":"8 1","pages":""},"PeriodicalIF":46.2,"publicationDate":"2025-11-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145583570","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}