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Twisted intramolecular charge transfer (TICT) based fluorescent probes and imaging agents 基于扭曲分子内电荷转移(TICT)的荧光探针和显像剂。
IF 39 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-21 DOI: 10.1039/D3CS01118F
Yueci Wu, Han-Min Wang, Xi-Le Hu, Yi Zang, Jia Li, Hai-Hao Han, Xiao-Peng He, Simon E. Lewis, Hanafy M. Ismail and Tony D. James

Twisted Intramolecular charge transfer (TICT)-based fluorescent probes are crucial in chemical sensing due to their sensitivity and specificity. These probes undergo conformational changes upon interacting with target analytes, resulting in measurable fluorescence responses. Their environment-dependent emission characteristics make them ideal for detecting variations in solvent polarity, microviscosity, and specific chemical species. Recent advances have expanded their applications to organic optoelectronics and non-linear optics. This review discusses the design principles, mechanisms, and applications of TICT-based probes, emphasizing their role in detecting cations, anions, and neutral molecules. We describe their advantages, such as fluorescence turn-on or turn-off responses and potential for ratiometric detection, which inherently corrects for interferences. Challenges in developing these probes, including fluorescence quantum yield and photostability, are also addressed. Potential directions for future research are highlighted, including the need for improved biocompatibility and multimodal imaging capabilities, with the aim of enhancing their utility in environmental monitoring, biomedical research, and clinical diagnostics.

基于扭曲分子内电荷转移(TICT)的荧光探针由于其灵敏度和特异性在化学传感中至关重要。这些探针在与目标分析物相互作用时经历构象变化,从而产生可测量的荧光响应。它们的环境依赖性发射特性使其成为检测溶剂极性,微粘度和特定化学物质变化的理想选择。近年来的进展已将其应用扩展到有机光电子学和非线性光学。本文综述了基于tict的探针的设计原理、机制和应用,重点介绍了其在检测阳离子、阴离子和中性分子中的作用。我们描述了它们的优点,如荧光打开或关闭响应和比例检测的潜力,它固有地纠正了干扰。还讨论了开发这些探针的挑战,包括荧光量子产率和光稳定性。强调了未来研究的潜在方向,包括改进生物相容性和多模态成像能力的需要,目的是提高它们在环境监测、生物医学研究和临床诊断中的应用。
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引用次数: 0
Symmetry breaking of single-atom catalysts in heterogeneous electrocatalysis: reactivity and configuration. 非均相电催化中单原子催化剂的对称性破缺:反应性和构型。
IF 46.2 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-21 DOI: 10.1039/d5cs00209e
Bin Wu,Zuohuan Chen,Yifan Ye,Justin Zhu Yeow Seow,Daniel Mandler,Adrian Fisher,Dingsheng Wang,Shaojun Guo,Zhichuan J Xu
Single-atom catalysts (SACs) have emerged as transformative materials in heterogeneous electrocatalysis, yet their conventional symmetric coordination environments often yield suboptimal catalytic efficacy. This review systematically examines the deliberate disruption of local symmetry as a powerful design strategy to precisely tailor the electronic properties of SACs. We categorize and analyze atomic-level modulation approaches, including strain-induced lattice distortion, defect-engineered coordination tailoring, and curvature-derived interfacial fields, demonstrating how these strategies effectively break the intrinsic symmetry of motifs such as M-N4. Our analysis reveals that such symmetry breaking redistributes electron density around the metal center, lifts orbital degeneracy, and optimizes the d-band center, leading to enhanced intermediate adsorption, accelerated reaction kinetics, and broken scaling relationships. Furthermore, these asymmetrically configured SACs exhibit improved stability through strengthened metal-support interactions. While significant progress has been made, we conclude that future efforts must address the challenges of atomic-level precision, stability under operation, and scalable synthesis to fully realize the potential of symmetry-broken SACs across various electrocatalytic applications, thereby establishing a new paradigm for the rational design of advanced electrocatalytic materials.
单原子催化剂(SACs)已成为多相电催化中的变革性材料,但其传统的对称配位环境往往产生不理想的催化效果。这篇综述系统地研究了故意破坏局部对称作为一种强大的设计策略,以精确地定制sac的电子特性。我们对原子级调制方法进行了分类和分析,包括应变诱导的晶格畸变、缺陷工程协调裁剪和曲率衍生的界面场,并展示了这些策略如何有效地打破M-N4等基元的固有对称性。我们的分析表明,这种对称破缺使金属中心周围的电子密度重新分布,提高了轨道简并,优化了d带中心,从而增强了中间吸附,加速了反应动力学,破坏了标度关系。此外,这些不对称结构的SACs通过加强金属-支撑相互作用表现出更好的稳定性。虽然已经取得了重大进展,但我们得出结论,未来的努力必须解决原子级精度,操作稳定性和可扩展合成的挑战,以充分实现对称破断SACs在各种电催化应用中的潜力,从而为合理设计先进的电催化材料建立新的范例。
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引用次数: 0
Towards greener-by-design fine chemicals. Part 2: technological frontiers 走向绿色设计的精细化学品。第二部分:技术前沿
IF 46.2 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-20 DOI: 10.1039/d5cs00930h
Theodore A. Gazis, Rodolfo I. Teixeira, Giulio Volpin, Ashish Yewale, Mert Can Ince, Mark J. Ford, Jan Harmsen, Marco Uboldi, Alice Melocchi, Mattia Sponchioni, Andrea Aramini, Renzo Luisi, Brahim Benyahia, Gianvito Vilé
Over the past three decades, the pharmaceutical and agrochemical sectors have embarked on a transformative journey towards greener-by-design processes, firmly rooted in the principles of green chemistry. Building on this foundation, green engineering frameworks have expanded the focus beyond environmental concerns to encompass product quality, economic viability, and the evolving demands of modern healthcare. At the heart of this transformation is continuous and smart manufacturing due to its capacity to reduce raw material use, waste, and energy consumption. While attention has understandably centered on replacing or refining conventional batch operations, the breadth of progress is far wider. Advanced analytics and digitization, as exemplified by AI-driven modeling, are nurturing the rise of “smart factories” that autonomously optimize performance in real time. A prime illustration lies in the purification of fine chemicals, where real-time analytics and advanced process control slash solvent requirements, an acute pollution hotspot, while ensuring consistent product quality. Meanwhile, 3D printing has introduced a genuinely disruptive dimension, challenging traditional notions of scale and location through on-demand, flexible production. In this piece, we explore how these converging technological frontiers lay the groundwork for the patient-centered, eco-conscious pharmaceutical and agrochemical facilities of the future.
在过去的三十年中,制药和农用化学品行业已经踏上了向绿色设计过程的变革之旅,坚定地植根于绿色化学的原则。在此基础上,绿色工程框架将关注点从环境问题扩展到产品质量、经济可行性和现代医疗保健不断变化的需求。这种转变的核心是连续和智能制造,因为它能够减少原材料使用、浪费和能源消耗。虽然人们的注意力集中在取代或改进传统的批量操作上是可以理解的,但进展的广度要大得多。以人工智能驱动的建模为例,先进的分析和数字化正在培育能够实时自主优化性能的“智能工厂”的兴起。一个典型的例子是精细化学品的净化,实时分析和先进的过程控制降低了对溶剂的要求,这是一个严重的污染热点,同时确保了一致的产品质量。与此同时,3D打印引入了一个真正具有颠覆性的维度,通过按需灵活生产,挑战了传统的规模和位置概念。在这篇文章中,我们探讨了这些融合的技术前沿如何为未来以患者为中心、具有生态意识的制药和农化设施奠定基础。
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引用次数: 0
Recent advances in high-entropy materials for efficient alkali metal-ion batteries 高效碱金属离子电池用高熵材料的研究进展
IF 39 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-20 DOI: 10.1039/D5CS00450K
Liping Duan, Yichen Du, Yijiang Liu, Haowei Tang, Chi Zhou, Dong Ha Kim, Zhiqun Lin and Xiaosi Zhou

Alkali metal-ion batteries (Li+/Na+/K+, AMIBs) are considered ideal choices for grid-scale energy storage systems due to their high energy density and long cycle life. However, issues such as insufficient structural stability of electrode materials and limited ion transport dynamics in electrolytes severely restrict their large-scale commercial applications. Notably, high-entropy design strategies characterized by four core effects—the high-entropy effect, lattice distortion effect, sluggish diffusion effect, and cocktail effect—have demonstrated remarkable transformative potential by synergistically enhancing the structural stability and ion/electron transport kinetics of materials, thereby significantly improving the electrochemical performance of AMIBs. In this review, we focus on the four core effects of high-entropy materials in AMIBs, highlighting their roles in enhancing the performance of cathode/anode materials, electrolytes, electrode/electrolyte interfaces, and full cells. We comprehensively summarize the current research progress and delve into advanced characterization techniques for high-entropy materials. In addition, this review offers a detailed summary of rational structural design strategies and fundamental guiding principles for high-entropy materials in efficient AMIBs. We hope that this review will inspire greater interest in the development of high-entropy AMIBs and pave the way for their future commercial applications.

碱金属离子电池(Li+/Na+/K+, amib)由于其高能量密度和长循环寿命而被认为是电网规模储能系统的理想选择。然而,电极材料结构稳定性不足、电解质中离子输运动力学受限等问题严重制约了其大规模商业应用。值得注意的是,以高熵效应、晶格畸变效应、缓慢扩散效应和鸡尾酒效应为核心效应的高熵设计策略通过协同提高材料的结构稳定性和离子/电子传递动力学,从而显着提高了AMIBs的电化学性能,显示出显著的变革潜力。在这篇综述中,我们重点介绍了高熵材料在AMIBs中的四个核心效应,重点介绍了它们在提高阴极/阳极材料、电解质、电极/电解质界面和满电池性能方面的作用。我们全面总结了目前的研究进展,并深入研究了高熵材料的先进表征技术。此外,本文还详细总结了高效amib中高熵材料的合理结构设计策略和基本指导原则。我们希望这篇综述将激发人们对高熵amib发展的更大兴趣,并为其未来的商业应用铺平道路。
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引用次数: 0
Recent advances in asymmetric bimetallic catalysis. 不对称双金属催化研究进展。
IF 46.2 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-19 DOI: 10.1039/d5cs00413f
Fang Wei,Jialin Qi,Xiangqing Jia,Zhenghu Xu
Asymmetric bimetallic catalysis has emerged as a powerful and efficient approach for the development of novel enantioselective transformations. By employing two metal centers with complementary reactivity, bimetallic catalysts enable dual substrate activation, stabilize reactive intermediates, and facilitate unique transformations with high enantioselectivity. This review summarizes recent significant advances in the field, including three different reaction modes: dual metal Lewis acid catalysis, transition-metal/metal Lewis acid catalysis, and dual transition-metal catalysis. By exploring the latest breakthroughs and providing a comprehensive outlook on the promising potential of asymmetric bimetallic catalysis, we aim to inspire further progress in this rapidly evolving area and highlight future opportunities for expanding its applications.
不对称双金属催化已成为发展新型对映选择性转化的一种强大而有效的方法。双金属催化剂通过采用两个具有互补反应活性的金属中心,使双底物活化,稳定反应中间体,并促进具有高对映选择性的独特转化。本文综述了近年来该领域的重要进展,包括三种不同的反应模式:双金属Lewis酸催化、过渡金属/金属Lewis酸催化和双过渡金属催化。通过探索不对称双金属催化的最新突破和对其前景的全面展望,我们的目标是激发这一快速发展领域的进一步进展,并强调扩大其应用的未来机会。
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引用次数: 0
Tailoring the dynamic nanocomposite hydrogels through surface-functionalized nanomaterials and interfacial crosslinking chemistry toward multifunctional biomedical and engineering applications. 通过表面功能化纳米材料和界面交联化学来定制动态纳米复合水凝胶,以实现多功能生物医学和工程应用。
IF 46.2 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-19 DOI: 10.1039/d5cs00975h
Yu-Chia Su,Grace Chen,Yi-Jhen Lai,Guo-Zen Song,Tai-Lin Wu,Yi-Cheun Yeh
Dynamic nanocomposite hydrogels (DNCHs) represent a cutting-edge class of materials characterized by their tunable architecture and stimuli-responsive behavior, making them particularly well-suited for applications that require mimicking the adaptive functionality of biological systems. A wide range of chemical strategies and design methodologies have been explored to engineer their structure-property-function relationships. In this review, we present a comprehensive analysis of recent developments in DNCHs, systematically organized into six material-centric categories, including metal-, metal oxide-, carbon-, ceramic-, polymer-, and metal-organic framework (MOF)-based nanomaterials. We examine surface functionalization techniques and interfacial crosslinking mechanisms that underpin DNCH fabrication, supported by representative examples that highlight their composition, interfacial chemistry, and functional performance. We also critically evaluate current challenges and highlight key research opportunities to inform and inspire future interdisciplinary efforts. Taken together, this review presents a cohesive and forward-looking framework to support the rational design, functional implementation, and collaborative advancement of next-generation DNCHs.
动态纳米复合水凝胶(DNCHs)代表了一类前沿材料,其特点是可调节的结构和刺激响应行为,使其特别适合需要模仿生物系统自适应功能的应用。已经探索了广泛的化学策略和设计方法来设计它们的结构-性能-功能关系。在这篇综述中,我们全面分析了DNCHs的最新发展,系统地分为六个以材料为中心的类别,包括金属基、金属氧化物基、碳基、陶瓷基、聚合物基和金属有机框架基(MOF)纳米材料。我们研究了支持DNCH制造的表面功能化技术和界面交联机制,并通过突出其组成,界面化学和功能性能的代表性例子进行了支持。我们还批判性地评估当前的挑战,并强调关键的研究机会,以告知和激励未来的跨学科努力。综上所述,本综述提出了一个具有凝聚力和前瞻性的框架,以支持下一代DNCHs的合理设计、功能实现和协作推进。
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引用次数: 0
Single-molecule quantum tunnelling sensors 单分子量子隧穿传感器
IF 46.2 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-18 DOI: 10.1039/d4cs00375f
Long Yi, Yuxin Yang, Biao-Feng Zeng, Xu Liu, Joshua B. Edel, Aleksandar P. Ivanov, Longhua Tang
Single-molecule sensors are pivotal tools for elucidating chemical and biological phenomena. Among these, quantum tunnelling sensors occupy a unique position, due to the exceptional sensitivity of tunnelling currents to sub-ångström variations in molecular structure and electronic states. This capability enables simultaneous sub-nanometre spatial resolution and sub-millisecond temporal resolution, allowing direct observation of dynamic processes that remain concealed in ensemble measurements. This review outlines the fundamental principles of electron tunnelling through molecular junctions and highlights the development of key experimental architectures, including mechanically controllable break junctions and scanning tunnelling microscopy-based approaches. Applications in characterising molecular conformation, supramolecular binding, chemical reactivity, and biomolecular function are critically examined. Furthermore, we discuss recent methodological advances in data interpretation, particularly the integration of statistical learning and machine learning techniques to enhance signal classification and improve throughput. This review highlights the transformative potential of quantum-tunnelling-based single-molecule sensors to advance our understanding of molecular-scale mechanisms and to guide the rational design of functional molecular devices and diagnostic platforms.
单分子传感器是阐明化学和生物现象的关键工具。其中,量子隧穿传感器占有独特的地位,因为隧穿电流对分子结构和电子状态的亚-ångström变化具有特殊的灵敏度。这种能力可以同时实现亚纳米空间分辨率和亚毫秒时间分辨率,从而可以直接观察隐藏在集合测量中的动态过程。本文概述了通过分子结的电子隧穿的基本原理,并重点介绍了关键实验结构的发展,包括机械可控断裂结和基于扫描隧道显微镜的方法。在表征分子构象、超分子结合、化学反应性和生物分子功能方面的应用被严格审查。此外,我们讨论了数据解释的最新方法进展,特别是统计学习和机器学习技术的集成,以增强信号分类和提高吞吐量。这篇综述强调了基于量子隧道的单分子传感器的变革潜力,以促进我们对分子尺度机制的理解,并指导功能分子器件和诊断平台的合理设计。
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引用次数: 0
Catalytic redox-neutral carboxylation with CO2 二氧化碳催化氧化还原-中性羧化反应
IF 39 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-18 DOI: 10.1039/D5CS00877H
Si-Shun Yan, Tian-Yu Gao, Yi Liu, Yi-Fei Chen, Jun-Ze Zuo, Qin-Fang Zhang, Lei Song, Wei Zhang, Jian-Heng Ye and Da-Gang Yu

CO2 is an attractive C1 building block for the construction of valuable chemicals from the standpoint of global sustainability. Recent years have witnessed the rapid development of diverse catalytic CO2 fixations into organic compounds. Among various transformations, the synthesis of carboxylic acids with CO2 through C–C bond formation is highly attractive due to the wide application of carboxylic acids in organic synthesis and industrial processes. The catalytic redox-neutral carboxylation of readily accessible starting materials with CO2 leads to valuable carboxylic acids with high atom economy and selectivity. In this review, we summarize the development of redox-neutral carboxylation with CO2 under different catalytic systems over the past two decades. The specifics are organized by the type of substrates reacting with CO2, including catalytic carboxylation of C–X (X = Sn, B, Zn, Si) bonds, C–H bonds and unsaturated substrates. In addition, the remaining challenges and future avenues for investigation are also presented to guide continued exploration of this emerging field.

从全球可持续性的角度来看,二氧化碳是一种有吸引力的C1构建块,用于构建有价值的化学品。近年来,各种催化CO2固定成有机化合物的方法发展迅速。在各种转化中,由于羧酸在有机合成和工业过程中的广泛应用,通过C-C键与CO2合成羧酸具有很高的吸引力。用CO2催化氧化还原-中性羧化反应制备具有高原子经济性和选择性的有价羧酸。本文综述了近二十年来不同催化体系下二氧化碳氧化还原-中性羧化反应的研究进展。具体是由与CO2反应的底物类型组织的,包括催化羧基化的C-X (X = Sn, B, Zn, Si)键,C-H键和不饱和底物。此外,还提出了剩余的挑战和未来的研究途径,以指导这一新兴领域的持续探索。
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引用次数: 0
Advanced Ah-level zinc metal batteries 先进的ah级锌金属电池
IF 46.2 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-18 DOI: 10.1039/d5cs00371g
Zequan Zhao, Qingquan Ye, Yangyang Liu, Bingan Lu, Shuquan Liang, Jiang Zhou
Aqueous zinc metal batteries (ZMBs) are emerging as promising candidates for large-scale energy storage due to their cost-effectiveness, intrinsic safety, and abundant resources. However, translating ZMBs from laboratory-scale prototypes to ampere-hour (Ah)-level practical systems remains challenging, limited by issues such as Zn dendrite growth, cathode dissolution, and the lack of scalable fabrication methods for high-mass-loading electrodes with efficient ion/electron transport. This review systematically outlines recent strategies to overcome these barriers by addressing materials, manufacturing, and cell configuration. From the material perspective, bulk and surface modifications of the Zn anode and cathode can improve electrochemical stability and capacity retention through crystal structure tuning and interface stabilization. In electrode fabrication, dry processing and hierarchical structuring have emerged as key methods to support high mass loadings while maintaining effective electron/ion transport. Further at the device level, innovations in cell configuration, like lamination, winding techniques etc., enable better structural integrity and electrochemical performance tailored to aqueous systems. By integrating material innovation, scalable processing, and optimized cell architecture, these developments chart a path toward practical Ah-level ZMBs. This review highlights a comprehensive framework to bridge the lab-to-market gap, guiding future efforts to realize safe, low-cost, and sustainable energy storage at scale.
水锌金属电池(zmb)由于其成本效益、内在安全性和丰富的资源而成为大规模储能的有希望的候选者。然而,将zmb从实验室规模的原型转化为安培小时(Ah)级的实际系统仍然具有挑战性,受到锌枝晶生长、阴极溶解以及缺乏具有高效离子/电子传输的高质量负载电极的可扩展制造方法等问题的限制。这篇综述系统地概述了通过解决材料、制造和电池配置来克服这些障碍的最新策略。从材料的角度来看,锌阳极和阴极的体积和表面改性可以通过晶体结构调整和界面稳定来提高电化学稳定性和容量保持。在电极制造中,干法加工和分层结构已成为支持高质量负载同时保持有效电子/离子传输的关键方法。在设备层面上,电池配置的创新,如层压、缠绕技术等,可以为水系统提供更好的结构完整性和电化学性能。通过整合材料创新、可扩展工艺和优化的单元结构,这些发展为实用的ah级zmb指明了道路。这篇综述强调了一个全面的框架,以弥合从实验室到市场的差距,指导未来实现安全、低成本和可持续的大规模能源储存。
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引用次数: 0
Layered tin halide perovskites in photovoltaics 层状卤化锡钙钛矿在光伏中的应用
IF 39 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-18 DOI: 10.1039/D5CS00560D
Mengqiong Zhu, Bhumika Chaudhary, Anamika Mishra, Michael Saliba and Jovana V. Milić

Tin-based halide perovskites are emerging as promising alternatives to traditional lead-based perovskites due to their lower bandgaps, decreased toxicity, and comparable chemical properties. These materials offer unique structural and functional benefits for optoelectronic applications and photovoltaics, particularly in their low-dimensional or layered (2D) forms. Recent advancements have improved the solar-to-electric power conversion efficiency of tin-based halide perovskites by relying on organic spacers to control crystallisation and stabilise the materials. The versatility of molecular compositions and structural tuning of layered tin halide perovskites makes them appealing for next-generation photovoltaic technologies. This review highlights the structural characteristics, synthetic methods, and properties of layered tin halide perovskites, providing a comprehensive overview and discussing future prospects for environmentally friendly perovskite photovoltaics.

锡基卤化物钙钛矿因其更低的带隙、更低的毒性和类似的化学性质而成为传统铅基钙钛矿的有前途的替代品。这些材料为光电应用和光伏发电提供了独特的结构和功能优势,特别是在它们的低维或层状(2D)形式。最近的进展已经提高了锡基卤化物钙钛矿的太阳能到电力的转换效率,依靠有机间隔物来控制结晶和稳定材料。层状卤化锡钙钛矿的分子组成和结构调整的多功能性使它们对下一代光伏技术具有吸引力。本文综述了层状卤化锡钙钛矿的结构特点、合成方法和性能,对环境友好型钙钛矿光伏技术进行了全面的综述和展望。
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引用次数: 0
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