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Ion transport mechanisms in covalent organic frameworks: implications for technology. 共价有机框架中的离子传输机制:对技术的影响。
IF 40.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-18 DOI: 10.1039/d4cs00409d
Wonmi Lee, Haochen Li, Zhilin Du, Dawei Feng

Covalent organic frameworks (COFs) have emerged as promising materials for ion conduction due to their highly tunable structures and excellent electrochemical stability. This review paper explores the mechanisms of ion conduction in COFs, focusing on how these materials facilitate ion transport across their ordered structures, which is crucial for applications such as solid electrolytes in batteries and fuel cells. We discuss the design strategies employed to enhance ion conductivity, including pore size optimization, functionalization with ionic groups, and the incorporation of solvent molecules and salts. Additionally, we examine the various applications of ion-conductive COFs, particularly in energy storage and conversion technologies, highlighting recent advancements and future directions in this field. This review paper aims to provide a comprehensive overview of the current state of research on ion-conductive COFs, offering insights into their potential to design highly ion-conductive COFs considering not only fundamental studies but also practical perspectives for advanced electrochemical devices.

共价有机框架(COFs)因其高度可调的结构和出色的电化学稳定性,已成为前景广阔的离子传导材料。本综述论文探讨了 COF 中的离子传导机制,重点关注这些材料如何促进离子在其有序结构中的传输,这对于电池和燃料电池中的固体电解质等应用至关重要。我们讨论了增强离子传导性的设计策略,包括孔径优化、离子基团官能化以及溶剂分子和盐的加入。此外,我们还探讨了离子导电 COF 的各种应用,尤其是在能量存储和转换技术中的应用,重点介绍了该领域的最新进展和未来方向。本综述论文旨在全面概述离子导电 COF 的研究现状,深入探讨设计高离子导电 COF 的潜力,不仅考虑到基础研究,还考虑到先进电化学器件的实用前景。
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引用次数: 0
Advancing H2O2 electrosynthesis: enhancing electrochemical systems, unveiling emerging applications, and seizing opportunities. 推进 H2O2 电合成:增强电化学系统,揭示新兴应用,抓住机遇。
IF 40.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-18 DOI: 10.1039/d4cs00412d
Zhiping Deng, Seung Joon Choi, Ge Li, Xiaolei Wang

Hydrogen peroxide (H2O2) is a highly desired chemical with a wide range of applications. Recent advancements in H2O2 synthesis center on the electrochemical reduction of oxygen, an environmentally friendly approach that facilitates on-site production. To successfully implement practical-scale, highly efficient electrosynthesis of H2O2, it is critical to meticulously explore both the design of catalytic materials and the engineering of other components of the electrochemical system, as they hold equal importance in this process. Development of promising electrocatalysts with outstanding selectivity and activity is a prerequisite for efficient H2O2 electrosynthesis, while well-configured electrolyzers determine the practical implementation of large-scale H2O2 production. In this review, we systematically summarize fundamental mechanisms and recent achievements in H2O2 electrosynthesis, including electrocatalyst design, electrode optimization, electrolyte engineering, reactor exploration, potential applications, and integrated systems, with an emphasis on active site identification and microenvironment regulation. This review also proposes new insights into the existing challenges and opportunities within this rapidly evolving field, together with perspectives on future development of H2O2 electrosynthesis and its industrial-scale applications.

过氧化氢(H2O2)是一种应用广泛的理想化学品。H2O2 合成的最新进展集中在氧的电化学还原上,这是一种有利于现场生产的环保方法。要成功实现实际规模的 H2O2 高效电合成,关键是要精心探索催化材料的设计和电化学系统其他组件的工程设计,因为它们在这一过程中具有同等重要的意义。开发具有出色选择性和活性的电催化剂是实现高效 H2O2 电合成的先决条件,而配置良好的电解槽则决定了大规模 H2O2 生产的实际实施。在这篇综述中,我们系统地总结了 H2O2 电合成的基本机制和最新成果,包括电催化剂设计、电极优化、电解质工程、反应器探索、潜在应用和集成系统,重点是活性位点识别和微环境调控。本综述还对这一快速发展领域的现有挑战和机遇提出了新的见解,并对 H2O2 电合成及其工业规模应用的未来发展提出了展望。
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引用次数: 0
Protein desulfurization and deselenization. 蛋白质脱硫和脱硒。
IF 40.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-16 DOI: 10.1039/d4cs00135d
Vincent Diemer, Eliott Roy, Vangelis Agouridas, Oleg Melnyk

Methods enabling the dechalcogenation of thiols or selenols have been investigated and developed for a long time in fields of research as diverse as the study of prebiotic chemistry, the engineering of fuel processing techniques, the study of biomolecule structures and function or the chemical synthesis of biomolecules. The dechalcogenation of thiol or selenol amino acids is nowadays a particularly flourishing area of research for being a pillar of modern chemical protein synthesis, when used in combination with thiol or selenol-based chemoselective peptide ligation chemistries. This review offers a comprehensive and scholarly overview of the field, emphasizing emerging trends and providing a detailed and critical mechanistic discussion of the dechalcogenation methods developed so far. Taking advantage of recently published reports, it also clarifies some unexpected desulfurization reactions that were observed in the past and for which no explanation was provided at the time. Additionally, the review includes a discussion on principal desulfurization methods within the framework of newly introduced green chemistry metrics and toolkits, providing a well-rounded exploration of the subject.

硫醇或硒醇的脱钙方法在生物前化学研究、燃料加工技术工程、生物大分子结构和功能研究或生物大分子化学合成等多个研究领域都得到了长期的研究和开发。如今,硫醇或硒酚氨基酸的脱钙化是一个特别蓬勃发展的研究领域,因为它是现代化学蛋白质合成的支柱,与基于硫醇或硒酚的化学选择性肽连接化学结合使用。这篇综述对这一领域进行了全面的学术综述,强调了新出现的趋势,并对迄今为止开发的脱钙方法进行了详细而严谨的机理讨论。本综述还利用最近发表的报告,对过去观察到的一些意想不到的脱硫反应进行了澄清,但当时并没有对这些反应做出解释。此外,该综述还包括在新引入的绿色化学指标和工具包框架内对主要脱硫方法的讨论,从而对该主题进行了全面的探讨。
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引用次数: 0
Rechargeable alkali metal-chlorine batteries: advances, challenges, and future perspectives. 可充电碱金属氯电池:进展、挑战和未来展望。
IF 40.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-15 DOI: 10.1039/d4cs00202d
Zehui Xie, Lidong Sun, Muhammad Sajid, Yuancheng Feng, Zhenshan Lv, Wei Chen

The emergence of Li-SOCl2 batteries in the 1970s as a high-energy-density battery system sparked considerable interest among researchers. However, limitations in the primary cell characteristics have restricted their potential for widespread adoption in today's sustainable society. Encouragingly, recent developments in alkali/alkaline-earth metal-Cl2 (AM-Cl2) batteries have shown impressive reversibility with high specific capacity and cycle performance, revitalizing the potential of SOCl2 batteries and becoming a promising technology surpassing current lithium-ion batteries. In this review, the emerging AM-Cl2 batteries are comprehensively summarized for the first time. The development history and advantages of Li-SOCl2 batteries are traced, followed by the critical working mechanisms for achieving high rechargeability. The design concepts of electrodes and electrolytes for AM-Cl2 batteries as well as key characterization techniques are also demonstrated. Furthermore, the current challenges and corresponding strategies, as well as future directions regarding the battery are systematically discussed. This review aims to deepen the understanding of the state-of-the-art AM-Cl2 battery technology and accelerate the development of practical AM-Cl2 batteries for next-generation high-energy storage systems.

20 世纪 70 年代,作为一种高能量密度电池系统,锂-SOCl2 电池的出现引发了研究人员的极大兴趣。然而,原电池特性的局限性限制了其在当今可持续发展社会中广泛应用的潜力。令人鼓舞的是,碱/碱土金属-Cl2(AM-Cl2)电池的最新发展显示出令人印象深刻的可逆性、高比容量和循环性能,重振了 SOCl2 电池的潜力,成为超越当前锂离子电池的一项前景广阔的技术。本综述首次对新兴的 AM-Cl2 电池进行了全面总结。文章追溯了锂-SOCl2 电池的发展历史和优势,随后介绍了实现高充电性能的关键工作机制。还展示了 AM-Cl2 电池电极和电解质的设计理念以及关键表征技术。此外,还系统地讨论了该电池目前面临的挑战、相应的策略以及未来的发展方向。本综述旨在加深对最先进的 AM-Cl2 电池技术的理解,并加速开发用于下一代高能量存储系统的实用 AM-Cl2 电池。
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引用次数: 0
Microbe-material hybrids for therapeutic applications. 用于治疗的微生物-材料混合物。
IF 40.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-15 DOI: 10.1039/d3cs00655g
Meng Chen, Lili Xia, Chenyao Wu, Zeyu Wang, Li Ding, Yujie Xie, Wei Feng, Yu Chen

As natural living substances, microorganisms have emerged as useful resources in medicine for creating microbe-material hybrids ranging from nano to macro dimensions. The engineering of microbe-involved nanomedicine capitalizes on the distinctive physiological attributes of microbes, particularly their intrinsic "living" properties such as hypoxia tendency and oxygen production capabilities. Exploiting these remarkable characteristics in combination with other functional materials or molecules enables synergistic enhancements that hold tremendous promise for improved drug delivery, site-specific therapy, and enhanced monitoring of treatment outcomes, presenting substantial opportunities for amplifying the efficacy of disease treatments. This comprehensive review outlines the microorganisms and microbial derivatives used in biomedicine and their specific advantages for therapeutic application. In addition, we delineate the fundamental strategies and mechanisms employed for constructing microbe-material hybrids. The diverse biomedical applications of the constructed microbe-material hybrids, encompassing bioimaging, anti-tumor, anti-bacteria, anti-inflammation and other diseases therapy are exhaustively illustrated. We also discuss the current challenges and prospects associated with the clinical translation of microbe-material hybrid platforms. Therefore, the unique versatility and potential exhibited by microbe-material hybrids position them as promising candidates for the development of next-generation nanomedicine and biomaterials with unique theranostic properties and functionalities.

微生物作为天然的生命物质,已成为医学领域的有用资源,可用于制造从纳米到宏观尺寸的微生物-材料混合体。微生物参与的纳米医学工程利用了微生物的独特生理属性,特别是其固有的 "生命 "特性,如缺氧倾向和制氧能力。利用这些显著特点与其他功能材料或分子相结合,可实现协同增效,为改善给药、特定部位治疗和加强治疗效果监测带来巨大希望,为提高疾病治疗效果提供了大量机会。本综述概述了生物医学中使用的微生物和微生物衍生物及其在治疗应用中的具体优势。此外,我们还阐述了构建微生物-材料混合物的基本策略和机制。我们详尽阐述了所构建的微生物-材料混合物的各种生物医学应用,包括生物成像、抗肿瘤、抗菌、抗炎和其他疾病治疗。我们还讨论了微生物-材料杂交平台在临床转化方面目前面临的挑战和前景。因此,微生物-材料混合物所表现出的独特多功能性和潜力使其成为开发具有独特治疗特性和功能的下一代纳米药物和生物材料的理想候选材料。
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引用次数: 0
Spin states of metal centers in electrocatalysis. 电催化中金属中心的自旋态。
IF 40.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-15 DOI: 10.1039/d3cs00913k
Yuwei Zhang, Qian Wu, Justin Zhu Yeow Seow, Yingjie Jia, Xiao Ren, Zhichuan J Xu

Understanding the electronic structure of active sites is crucial in efficient catalyst design. The spin state, spin configurations of d-electrons, has been frequently discussed recently. However, its systematic depiction in electrocatalysis is lacking. In this tutorial review, a comprehensive interpretation of the spin state of metal centers in electrocatalysts and its role in electrocatalysis is provided. This review starts with the basics of spin states, including molecular field theory, crystal field theory, and ligand field theory. It further introduces the differences in low spin, intermediate spin, and high spin, and intrinsic factors affecting the spin state. Popular characterization techniques and modeling approaches that can reveal the spin state, such as X-ray absorption microscopy, electron spin resonance spectroscopy, Mössbauer spectroscopy, and density functional theory (DFT) calculations, are introduced as well with examples from the literature. The examples include the most recent progress in tuning the spin state of metal centers for various reactions, e.g., the oxygen evolution reaction, oxygen reduction reaction, hydrogen evolution reaction, carbon dioxide reduction reaction, nitrogen reduction reaction, nitrate reduction reaction, and urea oxidation reaction. Challenges and potential implications for future research related to the spin state are discussed at the end.

了解活性位点的电子结构对于高效催化剂的设计至关重要。自旋态,即 d 电子的自旋构型,最近经常被讨论。然而,对其在电催化中的应用还缺乏系统的描述。本教程综述全面解读了电催化剂中金属中心的自旋态及其在电催化中的作用。本综述从自旋态的基础知识开始,包括分子场理论、晶体场理论和配体场理论。它进一步介绍了低自旋、中间自旋和高自旋的差异,以及影响自旋态的内在因素。此外,还介绍了能揭示自旋态的常用表征技术和建模方法,如 X 射线吸收显微镜、电子自旋共振光谱学、莫斯鲍尔光谱学和密度泛函理论(DFT)计算,并列举了文献中的实例。这些例子包括在各种反应中调整金属中心自旋态的最新进展,例如氧进化反应、氧还原反应、氢进化反应、二氧化碳还原反应、氮还原反应、硝酸盐还原反应和尿素氧化反应。最后讨论了与自旋态有关的未来研究面临的挑战和潜在影响。
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引用次数: 0
Progress and challenges in nitrous oxide decomposition and valorization. 氧化亚氮分解和利用的进展与挑战。
IF 40.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-15 DOI: 10.1039/d3cs00919j
Xuanhao Wu, Jiaxin Du, Yanxia Gao, Haiqiang Wang, Changbin Zhang, Runduo Zhang, Hong He, Gaoqing Max Lu, Zhongbiao Wu

Nitrous oxide (N2O) decomposition is increasingly acknowledged as a viable strategy for mitigating greenhouse gas emissions and addressing ozone depletion, aligning significantly with the UN's sustainable development goals (SDGs) and carbon neutrality objectives. To enhance efficiency in treatment and explore potential valorization, recent developments have introduced novel N2O reduction catalysts and pathways. Despite these advancements, a comprehensive and comparative review is absent. In this review, we undertake a thorough evaluation of N2O treatment technologies from a holistic perspective. First, we summarize and update the recent progress in thermal decomposition, direct catalytic decomposition (deN2O), and selective catalytic reduction of N2O. The scope extends to the catalytic activity of emerging catalysts, including nanostructured materials and single-atom catalysts. Furthermore, we present a detailed account of the mechanisms and applications of room-temperature techniques characterized by low energy consumption and sustainable merits, including photocatalytic and electrocatalytic N2O reduction. This article also underscores the extensive and effective utilization of N2O resources in chemical synthesis scenarios, providing potential avenues for future resource reuse. This review provides an accessible theoretical foundation and a panoramic vision for practical N2O emission controls.

人们日益认识到,氧化亚氮(N2O)分解是减少温室气体排放和解决臭氧消耗问题的可行策略,与联合国可持续发展目标(SDGs)和碳中和目标高度一致。为了提高处理效率并挖掘潜在的价值,最近的发展引入了新型一氧化二氮还原催化剂和途径。尽管取得了这些进展,但却缺乏全面的比较性综述。在本综述中,我们将从整体角度对 N2O 处理技术进行全面评估。首先,我们总结并更新了热分解、直接催化分解(deN2O)和选择性催化还原 N2O 的最新进展。研究范围扩展到新兴催化剂的催化活性,包括纳米结构材料和单原子催化剂。此外,我们还详细介绍了室温技术的机理和应用,包括光催化和电催化 N2O 还原技术,这些技术具有能耗低和可持续的优点。本文还强调了 N2O 资源在化学合成方案中的广泛而有效的利用,为未来的资源再利用提供了潜在的途径。这篇综述为实际的一氧化二氮排放控制提供了通俗易懂的理论基础和全景视野。
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引用次数: 0
Catalytic asymmetric synthesis of 1,2-diamines. 1,2 二胺的催化不对称合成。
IF 40.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-11 DOI: 10.1039/d3cs00379e
Francisco Foubelo, Carmen Nájera, Ma Gracia Retamosa, José M Sansano, Miguel Yus

The asymmetric catalytic synthesis of 1,2-diamines has received considerable interest, especially in the last ten years, due to their presence in biologically active compounds and their applications for the development of synthetic building blocks, chiral ligands and organocatalysts. Synthetic strategies based on C-N bond-forming reactions involve mainly (a) ring opening of aziridines and azabenzonorbornadienes, (b) hydroamination of allylic amines, (c) hydroamination of enamines and (d) diamination of olefins. In the case of C-C bond-forming reactions are included (a) the aza-Mannich reaction of imino esters, imino nitriles, azlactones, isocyano acetates, and isothiocyanates with imines, (b) the aza-Henry reaction of nitroalkanes with imines, (c) imine-imine coupling reactions, and (d) reductive coupling of enamines with imines, and (e) [3+2] cycloaddition with imines. C-H bond forming reactions include hydrogenation of CN bonds and C-H amination reactions. Other catalytic methods include desymmetrization reactions of meso-diamines.

由于 1,2-二胺在生物活性化合物中的存在,以及它们在合成构件、手性配体和有机催化剂开发中的应用,1,2-二胺的不对称催化合成在过去十年中受到了广泛关注。基于 C-N 键形成反应的合成策略主要涉及 (a) 氮丙啶和氮杂苯并降冰片二烯的开环,(b) 烯丙基胺的氢化,(c) 烯胺的氢化和 (d) 烯烃的二胺化。C-C 键形成反应包括:(a) 亚氨基酯、亚氨基腈、氮杂内酯、异氰基乙酸酯和异硫氰酸酯与亚胺的杂-曼尼希反应;(b) 硝基烷烃与亚胺的杂-亨利反应;(c) 亚胺-亚胺偶联反应;(d) 烯胺与亚胺的还原偶联反应;(e) 亚胺的[3+2]环加成反应。C-H 键形成反应包括 CN 键的氢化反应和 C-H 氨化反应。其他催化方法包括中二胺的非对称化反应。
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引用次数: 0
Navigating the landscape of enzyme design: from molecular simulations to machine learning. 酶设计的导航:从分子模拟到机器学习。
IF 40.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-11 DOI: 10.1039/d4cs00196f
Jiahui Zhou, Meilan Huang

Global environmental issues and sustainable development call for new technologies for fine chemical synthesis and waste valorization. Biocatalysis has attracted great attention as the alternative to the traditional organic synthesis. However, it is challenging to navigate the vast sequence space to identify those proteins with admirable biocatalytic functions. The recent development of deep-learning based structure prediction methods such as AlphaFold2 reinforced by different computational simulations or multiscale calculations has largely expanded the 3D structure databases and enabled structure-based design. While structure-based approaches shed light on site-specific enzyme engineering, they are not suitable for large-scale screening of potential biocatalysts. Effective utilization of big data using machine learning techniques opens up a new era for accelerated predictions. Here, we review the approaches and applications of structure-based and machine-learning guided enzyme design. We also provide our view on the challenges and perspectives on effectively employing enzyme design approaches integrating traditional molecular simulations and machine learning, and the importance of database construction and algorithm development in attaining predictive ML models to explore the sequence fitness landscape for the design of admirable biocatalysts.

全球环境问题和可持续发展呼唤精细化学品合成和废物价值化的新技术。作为传统有机合成的替代技术,生物催化技术备受关注。然而,要在浩瀚的序列空间中识别出具有令人钦佩的生物催化功能的蛋白质是一项挑战。最近,基于深度学习的结构预测方法(如 AlphaFold2)得到了不同计算模拟或多尺度计算的加强,在很大程度上扩展了三维结构数据库,实现了基于结构的设计。虽然基于结构的方法为特定位点的酶工程提供了启示,但并不适合大规模筛选潜在的生物催化剂。利用机器学习技术有效利用大数据开辟了加速预测的新时代。在此,我们回顾了基于结构和机器学习指导的酶设计方法和应用。我们还就有效利用传统分子模拟和机器学习相结合的酶设计方法所面临的挑战和前景,以及数据库建设和算法开发在获得预测性 ML 模型以探索序列适配性景观以设计理想的生物催化剂方面的重要性提出了自己的看法。
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引用次数: 0
Nature-inspired adhesive systems. 受大自然启发的粘合剂系统。
IF 40.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-10 DOI: 10.1039/d3cs00764b
Ming Li, Anran Mao, Qingwen Guan, Eduardo Saiz

Many organisms in nature thrive in intricate habitats through their unique bio-adhesive surfaces, facilitating tasks such as capturing prey and reproduction. It's important to note that the remarkable adhesion properties found in these natural biological surfaces primarily arise from their distinct micro- and nanostructures and/or chemical compositions. To create artificial surfaces with superior adhesion capabilities, researchers delve deeper into the underlying mechanisms of these captivating adhesion phenomena to draw inspiration. This article provides a systematic overview of various biological surfaces with different adhesion mechanisms, focusing on surface micro- and nanostructures and/or chemistry, offering design principles for their artificial counterparts. Here, the basic interactions and adhesion models of natural biological surfaces are introduced first. This will be followed by an exploration of research advancements in natural and artificial adhesive surfaces including both dry adhesive surfaces and wet/underwater adhesive surfaces, along with relevant adhesion characterization techniques. Special attention is paid to stimulus-responsive smart artificial adhesive surfaces with tunable adhesive properties. The goal is to spotlight recent advancements, identify common themes, and explore fundamental distinctions to pinpoint the present challenges and prospects in this field.

自然界中的许多生物通过其独特的生物粘附表面在错综复杂的栖息地中茁壮成长,为捕捉猎物和繁殖等任务提供便利。值得注意的是,这些天然生物表面所具有的显著粘附特性主要源于它们独特的微纳米结构和/或化学成分。为了创造出具有卓越粘附能力的人造表面,研究人员深入研究了这些迷人的粘附现象的内在机理,从中汲取灵感。本文系统概述了具有不同粘附机制的各种生物表面,重点介绍了表面的微纳米结构和/或化学成分,为人工表面的设计提供了原则。本文首先介绍了天然生物表面的基本相互作用和粘附模型。随后将探讨天然和人工粘附表面的研究进展,包括干粘附表面和湿/水下粘附表面,以及相关的粘附表征技术。特别关注具有可调粘合特性的刺激响应型智能人工粘合表面。其目的是聚焦最新进展,确定共同主题,探讨基本区别,从而明确该领域当前的挑战和前景。
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引用次数: 0
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