Accounts of materials research最新文献

{"title":"Constructing High-Performance Heterogeneous Catalysts through Interface Engineering on Metal–Organic Framework Platforms","authors":"Bo Li, Jian-Gong Ma, Peng Cheng","doi":"10.1021/accountsmr.4c00367","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00367","url":null,"abstract":"Heterogeneous catalysis has pushed the modern chemical industry to an unprecedented level of development, especially in the past century, where catalytic processes have made significant contributions to the prosperity of the global economy and the modernization of human lifestyles. 80% of chemical processes involve catalytic technology. From the production of fertilizers and the synthesis of high-performance polymers to the development of anticancer drugs, catalysts mediate the occurrence of these chemical processes. Developing efficient, stable, and low-energy heterogeneous catalysts is the key to a sustainable future. Most industrial heterogeneous catalysts typically load highly dispersed active components at the nanoscale onto porous solid supports, which have a large specific surface area. Among the numerous candidates for porous materials, the construction of high-performance heterogeneous catalyst systems through interface engineering on metal–organic framework (MOF) platforms has recently received great attention. Compared with traditional porous materials, MOFs provide a huge active interface for catalytic reactions due to their large specific surface area and porosity. Their extraordinary skeleton structure provides many possibilities for integrating various functional building blocks. At the same time, as crystalline materials with diverse structures, their well-defined atomically precise structure provides an ideal platform for customized design and synthesis of catalysts as well as in-depth exploration of the structure–activity relationship between the structure of catalyst and the catalytic performance. After more than a decade of development, interface engineering has played a significant role in the development of MOF-based heterogeneous catalysts. Therefore, it is timely to summarize the latest developments in this field, which will provide guidance for future research and achieve green, low-carbon, and sustainable modern industries.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"77 4 Pt 1 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143077143","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Why and How to Investigate Biological Materials Processing: A Cross-Disciplinary Approach for Inspiring Sustainable Materials Fabrication","authors":"Matthew J. Harrington","doi":"10.1021/accountsmr.4c00334","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00334","url":null,"abstract":"Enhancing the performance and sustainability of materials is a major challenge facing humanity. With nearly 400 million tons of plastics manufactured per year and plastic waste accumulation of 12 billion tons expected by 2050, the production and buildup of anthropogenic petroleum-based waste is a major threat to our global ecosystem. This impending environmental catastrophe demands alternative sustainable and circular routes for material production. Additionally, there is a need for new polymeric materials that possess properties not currently found in synthetic materials for various applications in biomedical engineering, soft robotics, flexible electronics, and more. Nature offers inspiration for solving both of these environmentally, economically, and socially impactful global issues. Indeed, living organisms, such as spiders and mussels, rapidly fabricate polymeric biological materials from biomolecular building blocks (e.g., proteins) under green, environmentally benign processing conditions. These materials exhibit properties that surpass many synthetic plastics (e.g., high toughness, self-healing, “smart” adaptability, underwater adhesion), providing a blueprint for how humans can develop sustainable fabrication practices for producing next-generation materials. There is now a solid understanding of the structure–function relationships defining the performance of many biological materials, with control of structural hierarchy from nanoscale to centimeter scale emerging as a common design feature. Yet, it has been extremely challenging to replicate this hierarchical structure and, thus, the relevant properties in synthetic materials. This is largely due to a poor understanding of how these materials are fabricated by living organisms. Indeed, elucidation of the physicochemical principles underlying the fabrication of these and similar materials is significantly hampered due to experimental challenges in following these dynamic processes at the relevant spatiotemporal scales. Here, I outline a cross-disciplinary experimental approach spanning organismal biology, molecular biology, biochemistry, physical chemistry, and materials science for extracting design principles from biofabrication processes. As a model system, I focus on the fabrication of the mussel byssus–a biopolymeric fibrous holdfast with outstanding properties (underwater adhesion, high toughness, self-healing capacity) that is an established archetype for sustainable bioinspired fibers, glues, composites, and coatings. Careful analysis combining traditional histology and biochemical approaches with advanced spectroscopic imaging (e.g, confocal Raman spectroscopy, FTIR spectroscopy, and micro X-ray fluorescence), tomographic approaches (e.g., micro-CT), and advanced electron microscopy (e.g., focused ion beam scanning electron microscopy (FIB-SEM)) have yielded deep insights into the byssus assembly process, highlighting the key role of fluid protein condensates (liquid crystals","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"59 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050133","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Why and How to Investigate Biological Materials Processing: A Cross-Disciplinary Approach for Inspiring Sustainable Materials Fabrication","authors":"Matthew J. Harrington*, ","doi":"10.1021/accountsmr.4c0033410.1021/accountsmr.4c00334","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00334https://doi.org/10.1021/accountsmr.4c00334","url":null,"abstract":"<p >Enhancing the performance and sustainability of materials is a major challenge facing humanity. With nearly 400 million tons of plastics manufactured per year and plastic waste accumulation of 12 billion tons expected by 2050, the production and buildup of anthropogenic petroleum-based waste is a major threat to our global ecosystem. This impending environmental catastrophe demands alternative sustainable and circular routes for material production. Additionally, there is a need for new polymeric materials that possess properties not currently found in synthetic materials for various applications in biomedical engineering, soft robotics, flexible electronics, and more. Nature offers inspiration for solving both of these environmentally, economically, and socially impactful global issues. Indeed, living organisms, such as spiders and mussels, rapidly fabricate polymeric biological materials from biomolecular building blocks (e.g., proteins) under green, environmentally benign processing conditions. These materials exhibit properties that surpass many synthetic plastics (e.g., high toughness, self-healing, “smart” adaptability, underwater adhesion), providing a blueprint for how humans can develop sustainable fabrication practices for producing next-generation materials. There is now a solid understanding of the structure–function relationships defining the performance of many biological materials, with control of structural hierarchy from nanoscale to centimeter scale emerging as a common design feature. Yet, it has been extremely challenging to replicate this hierarchical structure and, thus, the relevant properties in synthetic materials. This is largely due to a poor understanding of how these materials are fabricated by living organisms. Indeed, elucidation of the physicochemical principles underlying the fabrication of these and similar materials is significantly hampered due to experimental challenges in following these dynamic processes at the relevant spatiotemporal scales. Here, I outline a cross-disciplinary experimental approach spanning organismal biology, molecular biology, biochemistry, physical chemistry, and materials science for extracting design principles from biofabrication processes. As a model system, I focus on the fabrication of the mussel byssus–a biopolymeric fibrous holdfast with outstanding properties (underwater adhesion, high toughness, self-healing capacity) that is an established archetype for sustainable bioinspired fibers, glues, composites, and coatings. Careful analysis combining traditional histology and biochemical approaches with advanced spectroscopic imaging (e.g, confocal Raman spectroscopy, FTIR spectroscopy, and micro X-ray fluorescence), tomographic approaches (e.g., micro-CT), and advanced electron microscopy (e.g., focused ion beam scanning electron microscopy (FIB-SEM)) have yielded deep insights into the byssus assembly process, highlighting the key role of fluid protein condensates (liquid crys","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 3","pages":"294–305 294–305"},"PeriodicalIF":14.0,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143714036","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Molecule-Based Crystalline Adsorbents: Advancing Adsorption Theory and Storage/Separation Applications","authors":"Xue-Wen Zhang, Jie-Peng Zhang, Xiao-Ming Chen","doi":"10.1021/accountsmr.4c00316","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00316","url":null,"abstract":"As a simple and common physicochemical process, adsorption is the basis of storage, separation, and many other applications. Compared to conventional adsorbents, molecule-based crystalline materials show advantages of extremely rich and easily designable/synthesized/characterized structures as well as remarkable flexibility. The emergence of new adsorbent materials has brought forth both opportunities and challenges for adsorption theory and its applications.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"75 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143020942","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Molecule-Based Crystalline Adsorbents: Advancing Adsorption Theory and Storage/Separation Applications","authors":"Xue-Wen Zhang, Jie-Peng Zhang* and Xiao-Ming Chen, ","doi":"10.1021/accountsmr.4c0031610.1021/accountsmr.4c00316","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00316https://doi.org/10.1021/accountsmr.4c00316","url":null,"abstract":"<p >As a simple and common physicochemical process, adsorption is the basis of storage, separation, and many other applications. Compared to conventional adsorbents, molecule-based crystalline materials show advantages of extremely rich and easily designable/synthesized/characterized structures as well as remarkable flexibility. The emergence of new adsorbent materials has brought forth both opportunities and challenges for adsorption theory and its applications.</p><p >Focusing on the simplest applications of adsorption, i.e., storage and separation, this Account aims to analyze the representative adsorbent engineering strategies. First, we provide a brief introduction to conventional adsorption theory and the fundamental principles of adsorptive storage and separation applications. Following that, we discuss how the special structural characteristics of molecule-based crystalline adsorbents, especially their flexibility, provide new insights and directions.</p><p >According to the well-established adsorption theory, molecule-based crystalline porous materials offer not only exceptionally large pore volumes and specific surface areas but also a wide variety of adsorption sites with a tunable guest binding affinity. More importantly, the concentration and position of the adsorption sites can be engineered and straightforwardly visualized. By rationally tuning host–guest and guest–guest interactions, the adsorption isotherm shape can be regulated to increase working capacity and selectivity and even inverse selectivity to meet practical separation demands.</p><p >Inspired by the structural flexibility of molecule-based crystalline materials, we need to consider the structural transformations of host–guest systems in the adsorption processes, in not only the thermodynamic but also the kinetic aspects. Rational classification of the various types of flexibility or structural transformations is crucial for elucidating the structure–property relationships in these host–guest systems. As the most well-known type of flexibility, guest-induced crystal-to-crystal structural transformations are thermodynamically controlled and occur periodically at the equilibrium state, which can be conveniently and straightforwardly visualized by diffraction techniques. Particularly, the pore-opening action (nonporous-to-porous transformation) can offer exceptionally high working capacity and remarkable advantages in terms of thermal effects. In the matter of crystalline adsorbents, this flexibility can also be aperiodic, which can effectively address the coadsorption and leakage issues to give high adsorption selectivity and purification productivity. The structural flexibility of host–guest systems can also be kinetically controlled and occur at the nonequilibrium state (and aperiodically). Gating flexibility describes the transient structural transformations for diffusion of oversized guest molecules, which not only provides more comprehensive mechanisms and criteria","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 3","pages":"259–273 259–273"},"PeriodicalIF":14.0,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143714034","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Engineering Cellular Vesicles for Immunotherapy","authors":"Xinyu Lin,&nbsp;Ludan Yue,&nbsp;Ke Cheng and Lang Rao*,&nbsp;","doi":"10.1021/accountsmr.4c0036210.1021/accountsmr.4c00362","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00362https://doi.org/10.1021/accountsmr.4c00362","url":null,"abstract":"<p >Immunotherapy has become a crucial strategy for cancer and infectious diseases due to its ability to leverage the power of the immune system to combat diseases, particularly when conventional therapeutic options have been ineffective. Nonetheless, low immune response rates and immune-related adverse events (irAEs) remain significant challenges for immunotherapeutics. Therefore, there is an urgent need to develop new strategies for improving the immunotherapy. Extracellular vesicles (EVs), secreted by living cells, are small membrane-bound vesicles. Their size varies from 30 to 150 nm in diameter and can be found in various bodily fluids, including blood, tears, and breast milk. They have attracted extensive attention in immunotherapy due to their integral role in essential physiological and pathological processes. Despite their potential, EVs face limitations, including low productivity and high costs, hindering their clinical applications. These issues have recently been addressed with the advent of EV mimics. EV mimics are artificially produced nanoscale vesicles. Compared to EVs, they offer superior production efficiency while maintaining similar biological properties. EV mimics are obtained by physical methods from natural cells. Methods such as serial extrusion, sonication, and electroporation are now used to produce synthetic EV mimics, making them viable for immunotherapy applications. Building on this, we have developed various EV mimics from different cell sources for immunotherapy and engineering natural EVs and EV mimics using chemical and bioengineering strategies like biochemical conjugation, genetic engineering, and membrane hybridization. These engineered natural EVs and EV mimics have controllable immunomodulatory properties, capable of modulating (i.e., boosting or inhibiting) immunity for the treatment of cancer and infectious diseases.</p><p >In this Account, we categorize both natural EVs and synthetic EV mimics under the umbrella term “cellular vesicles (CVs)” due to their similar structural and functional characteristics. We focus on recent advancements of CVs for immunotherapy, primarily work from our research group, and then summarize three main CV preparation methods, highlighting the microfluidic method developed by our team, which enables stable and efficient preparation. Following that, we outline engineering strategies for CVs to guide researchers in selecting the methods according to their needs. Additionally, we detail our progress in using CVs for treating cancer and infectious diseases. Finally, potential challenges and our future direction for overcoming these obstacles are also discussed. This Account highlights the development of engineered CVs, offering valuable insights into engineering strategies of personalized CVs and shedding new light on the therapeutic potential of biomimetic nanomaterials for cancer and infectious diseases.</p>","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 3","pages":"327–339 327–339"},"PeriodicalIF":14.0,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143714033","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Engineering Cellular Vesicles for Immunotherapy","authors":"Xinyu Lin, Ludan Yue, Ke Cheng, Lang Rao","doi":"10.1021/accountsmr.4c00362","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00362","url":null,"abstract":"Immunotherapy has become a crucial strategy for cancer and infectious diseases due to its ability to leverage the power of the immune system to combat diseases, particularly when conventional therapeutic options have been ineffective. Nonetheless, low immune response rates and immune-related adverse events (irAEs) remain significant challenges for immunotherapeutics. Therefore, there is an urgent need to develop new strategies for improving the immunotherapy. Extracellular vesicles (EVs), secreted by living cells, are small membrane-bound vesicles. Their size varies from 30 to 150 nm in diameter and can be found in various bodily fluids, including blood, tears, and breast milk. They have attracted extensive attention in immunotherapy due to their integral role in essential physiological and pathological processes. Despite their potential, EVs face limitations, including low productivity and high costs, hindering their clinical applications. These issues have recently been addressed with the advent of EV mimics. EV mimics are artificially produced nanoscale vesicles. Compared to EVs, they offer superior production efficiency while maintaining similar biological properties. EV mimics are obtained by physical methods from natural cells. Methods such as serial extrusion, sonication, and electroporation are now used to produce synthetic EV mimics, making them viable for immunotherapy applications. Building on this, we have developed various EV mimics from different cell sources for immunotherapy and engineering natural EVs and EV mimics using chemical and bioengineering strategies like biochemical conjugation, genetic engineering, and membrane hybridization. These engineered natural EVs and EV mimics have controllable immunomodulatory properties, capable of modulating (i.e., boosting or inhibiting) immunity for the treatment of cancer and infectious diseases.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"38 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142992581","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Machine Learning for Prediction and Synthesis of Anion Exchange Membranes","authors":"Yongjiang Yuan,&nbsp;Pengda Fang,&nbsp;Han Yuan,&nbsp;Xiuyang Zou,&nbsp;Zhe Sun* and Feng Yan*,&nbsp;","doi":"10.1021/accountsmr.4c0038410.1021/accountsmr.4c00384","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00384https://doi.org/10.1021/accountsmr.4c00384","url":null,"abstract":"&lt;p &gt;Anion exchange membrane fuel cells (AEMFCs) and water electrolyzers (AEMWEs) play a crucial role in the utilization and production of hydrogen energy, offering significant potential for widespread application due to their high energy conversion efficiency and cost-effectiveness. Anion exchange membranes (AEMs) serve the dual purpose of gas isolation and the conduction of OH&lt;sup&gt;–&lt;/sup&gt; ions. However, the poor chemical stability, low ionic conductivity, and inadequate dimensional stability of AEMs hinder the development of AEM-based energy devices. AEMs exhibit a more intricate chemical structure than general polymers, primarily due to their complex composition and unique attributes. This complexity is attributed to varying chain lengths, degrees of branching, and copolymerization compositions. Furthermore, diverse ion types, ion distribution, ion exchange capacity, hydrophilic clusters, electrostatic interactions, and microphase morphology further complicate these characteristics. In the past decade, more than 5,000 references have been dedicated to obtaining high-performance AEMs. Despite the large amount of work conducted during this period, the performance of AEMs still falls short of meeting the actual needs. The trial-and-error method used in designing membrane structures has proven inefficient and costly. Machine learning, a data-driven computational method, leverages existing data and algorithms to predict yet-to-be-discovered properties of materials. Recently, our group and some researchers have utilized machine learning to expedite the process of material discovery and achieve accurate synthesis of high-performance AEMs.&lt;/p&gt;&lt;p &gt;In this Account, we summarize the state-of-the-art for the AEMs, encompassing the structure design of cations and polymer backbones, strategies to improve the ion conductivity, and challenges arising from the necessity to achieve a delicate equilibrium among high conductivity, alkaline stability, and dimensional stability. Furthermore, we conduct a comprehensive review of recent breakthroughs in machine learning, specifically analyzing their implications within the context of AEMs. We examine the two primary branches of machine learning, supervised and unsupervised learning, and summarize various machine learning models, discussing the applicability and limitations of different algorithms. It is particularly worth noting that machine learning has the capability to predict the various properties of AEMs, such as conductivity and alkaline stability, and it can even design the structure of AEMs in accordance with the specific performance requirements of energy devices. By effectively screening high-performance membrane structures from millions of unknown candidates, machine learning significantly reduces the development time and cost associated with AEMs. Consequently, this technological advancement accelerates the rapid progress of AEM-based energy devices. Finally, we highlight the current challenge and future ","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 3","pages":"352–365 352–365"},"PeriodicalIF":14.0,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143714031","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Machine Learning for Prediction and Synthesis of Anion Exchange Membranes","authors":"Yongjiang Yuan, Pengda Fang, Han Yuan, Xiuyang Zou, Zhe Sun, Feng Yan","doi":"10.1021/accountsmr.4c00384","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00384","url":null,"abstract":"Anion exchange membrane fuel cells (AEMFCs) and water electrolyzers (AEMWEs) play a crucial role in the utilization and production of hydrogen energy, offering significant potential for widespread application due to their high energy conversion efficiency and cost-effectiveness. Anion exchange membranes (AEMs) serve the dual purpose of gas isolation and the conduction of OH^– ions. However, the poor chemical stability, low ionic conductivity, and inadequate dimensional stability of AEMs hinder the development of AEM-based energy devices. AEMs exhibit a more intricate chemical structure than general polymers, primarily due to their complex composition and unique attributes. This complexity is attributed to varying chain lengths, degrees of branching, and copolymerization compositions. Furthermore, diverse ion types, ion distribution, ion exchange capacity, hydrophilic clusters, electrostatic interactions, and microphase morphology further complicate these characteristics. In the past decade, more than 5,000 references have been dedicated to obtaining high-performance AEMs. Despite the large amount of work conducted during this period, the performance of AEMs still falls short of meeting the actual needs. The trial-and-error method used in designing membrane structures has proven inefficient and costly. Machine learning, a data-driven computational method, leverages existing data and algorithms to predict yet-to-be-discovered properties of materials. Recently, our group and some researchers have utilized machine learning to expedite the process of material discovery and achieve accurate synthesis of high-performance AEMs.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"13 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142989125","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Photoresponsive Coordination Polymer Single Crystal Platforms: Design and Applications","authors":"Qi Liu,&nbsp;Pierre Braunstein and Jian-Ping Lang*,&nbsp;","doi":"10.1021/accountsmr.4c0032510.1021/accountsmr.4c00325","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00325https://doi.org/10.1021/accountsmr.4c00325","url":null,"abstract":"&lt;p &gt;The concept of photoresponsive coordination polymer (CP) single crystal platforms (CPSCPs) is based on photoresponsive olefin CP single crystals, which can undergo photocycloaddition reactions under light irradiation through a single-crystal-to-single-crystal (SCSC) transformation. Taking advantage of the coordination of olefin ligands to metal ions of Zn&lt;sup&gt;2+&lt;/sup&gt;, Cd&lt;sup&gt;2+&lt;/sup&gt;, etc., a pair of C═C double bonds is positioned adjacent to each other in space at a suitable distance and orientation to allow [2 + 2] photocycloaddition triggered by UV–vis irradiation, affording cyclobutanes in the CPs. The single crystal nature of CPs allows their structures to be determined by X-ray diffraction, providing details of the arrangements in space of the C═C double bonds. These CPs are promising platforms for the synthesis of organic molecules, such as cyclobutanes and derivatives, with high regioselectivity and stereoselectivity without any catalyst. The [2 + 2] photocycloaddition reactions may induce structural modifications like expansion or shrinking of unit cells, resulting in macroscopic changes (e.g., cracking, bending, etc.) of the whole CP single crystals and leading to changes in chemical and physical properties. Applications take advantage of their optical properties, including luminescence and absorption, and allow the detection of guest molecules and photomechanical motions. Although much effort has been devoted to such studies, it remains challenging to develop systematic investigations aiming at increasing the diversity of CPs and properties to meet practical needs. Moreover, more efficient methods are desirable to investigate the reaction mechanisms in the solid state and monitor the structural changes occurring during the process.&lt;/p&gt;&lt;p &gt;In this Account, we introduce our research on the design and applications of photoresponsive CPSCPs. It is divided into three parts. First, the design and construction of various CPs with different olefin ligands are discussed. Through a suitable and sometimes sophisticated choice of metal ions and auxiliary carboxylate ligands, these olefin ligands meet the requirements to undergo [2 + 2] photocycloaddition reactions in CP structures, allowing for the precise synthesis of cyclobutanes and their derivatives. These compounds could be subsequently extracted from the CPs to give pure organic products. Second, we introduce new strategies, such as a combination of single crystal X-ray diffraction (SCXRD) with thermal/phototreatments of CPs and in situ fluorescence spectroscopy, to monitor the structural changes occurring on the olefin ligands during the reaction. Furthermore, the fast stepwise photoreaction could also be visualized with high resolution. These data significantly strengthen our understanding of solid-state [2 + 2] photocycloaddition reactions in CPs. Third, applications of photoresponsive CPs are described, which focus on optical and photoinduced mechanical properties. Considering the o","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 2","pages":"183–194 183–194"},"PeriodicalIF":14.0,"publicationDate":"2025-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143507914","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}