Chemical Society Reviews最新文献

{"title":"Carbonaceous materials in structural dimensions for advanced oxidation processes","authors":"Yunpeng Wang, Ya Liu, Huayang Zhang, Xiaoguang Duan, Jun Ma, Hongqi Sun, Wenjie Tian, Shaobin Wang","doi":"10.1039/d4cs00338a","DOIUrl":"https://doi.org/10.1039/d4cs00338a","url":null,"abstract":"Carbonaceous materials have attracted extensive research and application interests in water treatment owing to their advantageous structural and physicochemical properties. Despite the significant interest and ongoing debates on the mechanisms through which carbonaceous materials facilitate advanced oxidation processes (AOPs), a systematic summary of carbon materials across all dimensions (0D–3D nanocarbon to bulk carbon) in various AOP systems remains absent. Addressing this gap, the current review presents a comprehensive analysis of various carbon/oxidant systems, exploring carbon quantum dots (0D), nanodiamonds (0D), carbon nanotubes (1D), graphene derivatives (2D), nanoporous carbon (3D), and biochar (bulk 3D), across different oxidant systems: persulfates (peroxymonosulfate/peroxydisulfate), ozone, hydrogen peroxide, and high-valent metals (Mn(<small>VII</small>)/Fe(<small>VI</small>)). Our discussion is anchored on the identification of active sites and elucidation of catalytic mechanisms, spanning both radical and nonradical pathways. By dissecting catalysis-related factors such as sp<small>²</small>/sp<small>³</small> C, defects, and surface functional groups that include heteroatoms and oxygen groups in different carbon configurations, this review aims to provide a holistic understanding of the catalytic nature of different dimensional carbonaceous materials in AOPs. Furthermore, we address current challenges and underscore the potential for optimizing and innovating water treatment methodologies through the strategic application of carbon-based catalysts. Finally, prospects for future investigations and the associated bottlenecks are proposed.","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":"77 1","pages":""},"PeriodicalIF":46.2,"publicationDate":"2025-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143077374","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":"Enabling high-performance multivalent metal-ion batteries: current advances and future prospects.","authors":"Asif Mahmood, Zhe Bai, Tan Wang, Yaojie Lei, Shijian Wang, Bing Sun, Hajra Khan, Karim Khan, Kening Sun, Guoxiu Wang","doi":"10.1039/d4cs00929k","DOIUrl":"https://doi.org/10.1039/d4cs00929k","url":null,"abstract":"<p><p>The battery market is primarily dominated by lithium technology, which faces severe challenges because of the low abundance and high cost of lithium metal. In this regard, multivalent metal-ion batteries (MVIBs) enabled by multivalent metal ions (<i>e.g.</i> Zn²⁺, Mg²⁺, Ca²⁺, Al³⁺, <i>etc.</i>) have received great attention as an alternative to traditional lithium-ion batteries (Li-ion batteries) due to the high abundance and low cost of multivalent metals, high safety and higher volumetric capacities. However, the successful application of these battery chemistries requires careful control over electrode and electrolyte chemistries due to the higher charge density and slower kinetics of multivalent metal ions, structural instability of the electrode materials, and interfacial resistance, <i>etc.</i> This review comprehensively explores the recent advancements in electrode and electrolyte materials as well as separators for MVIBs, highlighting the potential of MVIBs to outperform Li-ion batteries regarding cost, energy density and safety. The review first summarizes the recent progress and fundamental charge storage mechanism in several MVIB chemistries, followed by a summary of major challenges. Then, a thorough account of the recently proposed methodologies is given including progress in anode/cathode design, electrolyte modifications, transition to semi-solid- and solid-state electrolytes (SSEs), modifications in separators as well as a description of advanced characterization tools towards understanding the charge storage mechanism. The review also accounts for the recent trend of using artificial intelligence in battery technology. The review concludes with a discussion on prospects, emphasizing the importance of material innovation and sustainability. Overall, this review provides a detailed overview of the current state and future directions of MVIB technology, underscoring its significance in advancing next-generation energy storage solutions.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" ","pages":""},"PeriodicalIF":40.4,"publicationDate":"2025-01-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143062620","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":"Models and simulations of structural DNA nanotechnology reveal fundamental principles of self-assembly","authors":"Alexander Cumberworth, Aleks Reinhardt","doi":"10.1039/d4cs01095g","DOIUrl":"https://doi.org/10.1039/d4cs01095g","url":null,"abstract":"DNA is not only a centrally important molecule in biology: the specificity of bonding that allows it to be the primary information storage medium for life has also allowed it to become one of the most promising materials for designing intricate, self-assembling structures at the nanoscale. While the applications of these structures are both broad and highly promising, the self-assembly process itself has attracted interest not only for the practical applications of designing structures with more efficient assembly pathways, but also due to a desire to understand the principles underlying self-assembling systems more generally, of which DNA-based systems provide intriguing and unique examples. Here, we review the fundamental physical principles that underpin the self-assembly process in the field of DNA nanotechnology, with a specific focus on simulation and modelling and what we can learn from them. In particular, we compare and contrast DNA origami and bricks and briefly outline other approaches, with an overview of concepts such as cooperativity, nucleation and hysteresis; we also explain how nucleation barriers can be controlled and why they can be helpful in ensuring error-free assembly. While high-resolution models may be needed to obtain accurate system-specific properties, often very simple coarse-grained models are sufficient to extract the fundamentals of the underlying physics and can enable us to gain deep insight. By combining experimental and simulation approaches to understand the details of the self-assembly process, we can optimise its yields and fidelity, which may in turn facilitate its use in practical applications.","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":"20 1","pages":""},"PeriodicalIF":46.2,"publicationDate":"2025-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143055647","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":"Dynamic regulation of ferroelectric polarization using external stimuli for efficient water splitting and beyond","authors":"Sundaram Chandrasekaran, Qingping Wang, Qiong Liu, Huihui Wang, Dingrong Qiu, Huidan Lu, Yongping Liu, Chris Bowen, Haitao Huang","doi":"10.1039/d4cs01322k","DOIUrl":"https://doi.org/10.1039/d4cs01322k","url":null,"abstract":"Establishing and regulating the ferroelectric polarization in ferroelectric nano-scale catalysts has been recognized as an emerging strategy to advance water splitting reactions, with the merits of improved surface charge density, high charge transfer rate, increased electronic conductivity, the creation of real active sites, and optimizing the chemisorption energy. As a result, engineering and tailoring the ferroelectric polarization induced internal electric field provides significant opportunities to improve the surface and electronic characteristics of catalysts, thereby enhancing the water splitting reaction kinetics. In this review, an interdisciplinary and comprehensive summary of recent advancements in the construction, characterization, engineering and regulation of the polarization in ferroelectric-based catalysts for water splitting is provided, by exploiting a variety of external stimuli. This review begins with a detailed overview of the classification, benefits, and identification methodologies of the ferroelectric polarization induced internal electric field; this offers significant insights for an in-depth analysis of ferroelectric-based catalysts. Subsequently, we explore the underlying structure–activity relationships for regulating the ferroelectric polarization using a range of external stimuli which include mechanical, magnetic, and thermal fields to achieve efficient water splitting, along with a combination of two or more fields. The review then highlights emerging strategies for multi-scale design and theoretical prediction of the relevant factors to develop highly promising ferroelectric catalysts for efficient water splitting. Finally, we present the challenges and perspectives on the potential research avenues in this fascinating and new field. This review therefore delivers an in-depth examination of the strategies to engineer the ferroelectric polarization for the next-generation of water electrolysis devices, systems and beyond.","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":"30 1","pages":""},"PeriodicalIF":46.2,"publicationDate":"2025-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143055649","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":"Quantum life science: biological nano quantum sensors, quantum technology-based hyperpolarized MRI/NMR, quantum biology, and quantum biotechnology.","authors":"Hiroshi Yukawa, Hidetoshi Kono, Hitoshi Ishiwata, Ryuji Igarashi, Yoichi Takakusagi, Shigeki Arai, Yu Hirano, Tetsuya Suhara, Yoshinobu Baba","doi":"10.1039/d4cs00650j","DOIUrl":"https://doi.org/10.1039/d4cs00650j","url":null,"abstract":"<p><p>The emerging field of quantum life science combines principles from quantum physics and biology to study fundamental life processes at the molecular level. Quantum mechanics, which describes the properties of small particles, can help explain how quantum phenomena such as tunnelling, superposition, and entanglement may play a role in biological systems. However, capturing these effects in living systems is a formidable challenge, as it involves dealing with dissipation and decoherence caused by the surrounding environment. We overview the current status of the quantum life sciences from technologies and topics in quantum biology. Technologies such as biological nano quantum sensors, quantum technology-based hyperpolarized MRI/NMR, high-speed 2D electronic spectrometers, and computer simulations are being developed to address these challenges. These interdisciplinary fields have the potential to revolutionize our understanding of living organisms and lead to advancements in genetics, molecular biology, medicine, and bioengineering.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" ","pages":""},"PeriodicalIF":40.4,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143051084","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":"Behavior, mechanisms, and applications of low-concentration CO2 in energy media","authors":"Minghai Shen, Wei Guo, Lige Tong, Li Wang, Paul K. Chu, Sibudjing Kawi, Yulong Ding","doi":"10.1039/d4cs00574k","DOIUrl":"https://doi.org/10.1039/d4cs00574k","url":null,"abstract":"This review explores the behavior of low-concentration CO<small>₂</small> (LCC) in various energy media, such as solid adsorbents, liquid absorbents, and catalytic surfaces. It delves into the mechanisms of diffusion, adsorption, and catalytic reactions, while analyzing the potential applications and challenges of these properties in technologies like air separation, compressed gas energy storage, and CO<small>₂</small> catalytic conversion. Given the current lack of comprehensive analyses, especially those encompassing multiscale studies of LCC behavior, this review aims to provide a theoretical foundation and data support for optimizing CO<small>₂</small> capture, storage, and conversion technologies, as well as guidance for the development and application of new materials. By summarizing recent advancements in LCC separation techniques (<em>e.g.</em>, cryogenic air separation and direct air carbon capture) and catalytic conversion technologies (including thermal catalysis, electrochemical catalysis, photocatalysis, plasma catalysis, and biocatalysis), this review highlights their importance in achieving carbon neutrality. It also discusses the challenges and future directions of these technologies. The findings emphasize that advancing the efficient utilization of LCC not only enhances CO<small>₂</small> reduction and resource utilization efficiency, promoting the development of clean energy technologies, but also provides an economically and environmentally viable solution for addressing global climate change.","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":"114 1","pages":""},"PeriodicalIF":46.2,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143044325","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":"Catalytic asymmetric photocycloaddition reactions mediated by enantioselective radical approaches","authors":"Yanli Yin, Mengdi You, Xiangtao Li, Zhiyong Jiang","doi":"10.1039/d5cs00019j","DOIUrl":"https://doi.org/10.1039/d5cs00019j","url":null,"abstract":"The use of olefins in the construction of cyclic compounds represents a powerful strategy for advancing the pharmaceutical industry. Photocycloaddition has attracted significant interest from chemists due to its ability to exploit simple and readily available olefins along with their reaction patterns under mild conditions. Moreover, the sustainable and versatile pathways for generating highly reactive intermediates can greatly enrich both substrate diversity and reaction patterns. As a result, numerous photocycloaddition reactions have been successfully developed, particularly asymmetric [2+2], [3+2], and [4+2] photocycloadditions mediated by enantioselective radical approaches, achieving remarkable enantioselectivities. This review offers a comprehensive overview of this rapidly evolving field, organizing the discussion into three distinct reaction types that facilitate the construction of enantioenriched derivatives of cyclobutanes, cyclopentanes, and cyclohexanes. Emphasis is placed on analyzing and summarizing established strategies aimed at circumventing the challenges posed by racemic background transformations. Additionally, the exploration of asymmetric [3+2] and [4+2] photocycloaddition reactions will be interwoven with a detailed discussion of the various substrate types involved. This systematic framework seeks to enhance understanding of the strategies employed to manage the high reactivity of radicals while achieving high enantioselectivity. Importantly, it aims to guide readers in identifying uncharted radical-based cycloaddition pathways, which possess significant potential to broaden the diversity of complex cyclic molecules.","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":"4 1","pages":""},"PeriodicalIF":46.2,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143044323","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":"Negative gas adsorption transitions and pressure amplification phenomena in porous frameworks","authors":"Simon Krause, Jack D. Evans, Volodymyr Bon, Irena Senkovska, François-Xavier Coudert, Gulliaume Maurin, Eike Brunner, Philip L. Llewellyn and Stefan Kaskel","doi":"10.1039/D4CS00555D","DOIUrl":"10.1039/D4CS00555D","url":null,"abstract":"<p >Nanoporous solids offer a wide range of functionalities for industrial, environmental, and energy applications. However, only a limited number of porous materials are responsive, <em>i.e.</em> the nanopore dynamically alters its size and shape in response to external stimuli such as temperature, pressure, light or the presence of specific molecular stimuli adsorbed inside the voids deforming the framework. Adsorption-induced structural deformation of porous solids can result in unique counterintuitive phenomena. Negative gas adsorption (NGA) is such a phenomenon which describes the spontaneous release of gas from an “overloaded” nanoporous solid <em>via</em> adsorption-induced structural contraction leading to total pressure amplification (PA) in a closed system. Such pressure amplifying materials may open new avenues for pneumatic system engineering, robotics, damping, or micromechanical actuators. In this review we illustrate the discovery of NGA in DUT-49, a mesoporous metal–organic framework (MOF), and the subsequent examination of conditions for its observation leading to a rationalization of the phenomenon. We outline the development of decisive experimental and theoretical methods required to establish the mechanism of NGA and derive key criteria for observing NGA in other porous solids. We demonstrate the application of these design principles in a series of DUT-49-related model compounds of which several also exhibit NGA. Furthermore, we provide an outlook towards applying NGA as a pressure amplification material and discuss possibilities to discover novel NGA materials and other counterintuitive adsorption phenomena in porous solids in the future.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" 3","pages":" 1251-1267"},"PeriodicalIF":40.4,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/cs/d4cs00555d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143044326","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":"Thermodynamic regulation of carbon dioxide capture by functionalized ionic liquids","authors":"Zhenyu Zhao, Kaili Wang, Han Tao, Zhaowei Zhang, Wenjun Lin, Qiaoxin Xiao, Lili Jiang, Haoran Li and Congmin Wang","doi":"10.1039/D4CS00972J","DOIUrl":"10.1039/D4CS00972J","url":null,"abstract":"<p >Carbon dioxide capture has attracted worldwide attention because CO<small>₂</small> emissions cause global warming and exacerbate climate change. Ionic liquids (ILs) have good application prospects in carbon capture due to their excellent properties, which provide a new chance to develop efficient and reversible carbon capture systems. This paper reviews the recent progress in CO<small>₂</small> chemical absorption by ILs, such as N-site, O-site, C-site, and multi-site functionalized ILs. The application of thermodynamic regulation methods in CO<small>₂</small> capture is discussed in detail. Among them, the methods of enthalpy regulation are mainly introduced, for which different regulatory targets are proposed for single sites and multiple sites. Furthermore, the strategies of achieving entropy compensation through the design of spatial configurations are discussed. Particular attention is paid to the application of thermodynamic regulation in direct air capture (DAC) due to its great significance. The methods to improve the absorption kinetics are also outlined. Finally, the future development of carbon capture by functionalized ILs is proposed.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" 4","pages":" 2091-2126"},"PeriodicalIF":40.4,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143044324","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":"Influence of π–π interactions on organic photocatalytic materials and their performance†","authors":"Liquan Jing, Pandeng Li, Zheng Li, Dongling Ma and Jinguang Hu","doi":"10.1039/D4CS00029C","DOIUrl":"10.1039/D4CS00029C","url":null,"abstract":"<p >Currently, organic photocatalyst-based photocatalysis has garnered significant attention as an environmentally friendly and sustainable reaction system due to the preferable structural flexibility and adjustable optoelectronic features of organic photocatalysts. In addition, π–π interactions, as one of the common non-bonded interactions, play an important role in the structure and property adjustments of organic photocatalysts due to their unique advantages in modulating the electronic structure, facilitating charge migration, and influencing interfacial reactions. However, studies summarizing the relationship between the π–π interactions of organic photocatalysts and their photocatalytic performance are still rare. Therefore, in this review, we introduced the types of π–π interactions, characterization techniques, and different types of organic photocatalytic materials. Then, the influence of π–π interactions on photocatalysis and the modification strategies of π–π interactions were summarized. Finally, we discussed their influence on photocatalytic performance in different photocatalytic systems and analyzed the challenges and prospects associated with harnessing π–π interactions in photocatalysis. The review provides a clear map for understanding π–π interaction formation mechanism and its application in organic photocatalysts, offering useful guidance for researchers in this field.</p>","PeriodicalId":68,"journal":{"name":"Chemical Society Reviews","volume":" 4","pages":" 2054-2090"},"PeriodicalIF":40.4,"publicationDate":"2025-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/cs/d4cs00029c?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143027059","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}