Accounts of materials research最新文献

{"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, Pierre Braunstein, Jian-Ping Lang","doi":"10.1021/accountsmr.4c00325","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00325","url":null,"abstract":"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 Zn²⁺, Cd²⁺, 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.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"48 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142940550","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}

{"title":"Pore Engineering in Metal–Organic Frameworks for Enhanced Hydrocarbon Adsorption and Separation","authors":"Xiao-Jing Xie,&nbsp;Min-Yi Zhou,&nbsp;Heng Zeng*,&nbsp;Weigang Lu* and Dan Li*,&nbsp;","doi":"10.1021/accountsmr.4c0033610.1021/accountsmr.4c00336","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00336https://doi.org/10.1021/accountsmr.4c00336","url":null,"abstract":"&lt;p &gt;The separation and purification of hydrocarbons are crucially important processes in the petrochemical industry, as they are essential for producing high-quality chemicals and fuels. However, traditional thermal-driven separation practices, such as cryogenic distillation, are notoriously energy-intensive, accounting for a notable portion of the energy consumption in industrial operations. This has spurred the exploration and development of low-energy and sustainable alternative separation technologies, among which adsorption/desorption-based separation with porous materials has gained significant attention. Metal–organic frameworks (MOFs) are emerging as ideal porous materials for hydrocarbon separation due to their exceptional porosity and structural tunability. This Account delves into the latest advancements in microporous MOFs for hydrocarbon separation, categorizing them based on their pore structures: single array, tandem array, and orthogonal array. Single-array MOFs feature uniformly arranged channel-like pores along the axial direction, facilitating the incorporation of binding sites on the pore surfaces. One notable functional group used in these applications is open metal sites (OMSs), which can engage in strong metal-π interactions with unsaturated hydrocarbons such as acetylene. For example, JNU-1 demonstrates increased binding energy with the increasing pressure of acetylene due to the induce-fit effect, where framework contraction behavior is triggered by its OMSs. JNU-4 offers two binding sites per metal center for acetylene molecules, greatly improving the adsorption capacity. On the other hand, introducing low-polarity groups, as seen in JNU-6-CH&lt;sub&gt;3&lt;/sub&gt;, can effectively enhance the separation performance in favor of alkanes while maintaining structural integrity under humid conditions. Another methyl group-modified MOF, JNU-5-CH&lt;sub&gt;3&lt;/sub&gt;, exhibits an acetylene-triggered gate-opening effect due to the multiple supramolecular interactions with acetylene. Tandem-array MOFs provide enhanced selectivity and adsorption capacity through the interconnection of spacious cavities with narrow apertures. For instance, JNU-2 with pore-channel interconnected structure exhibits improved separation efficiency for C&lt;sub&gt;2&lt;/sub&gt;H&lt;sub&gt;6&lt;/sub&gt;/C&lt;sub&gt;2&lt;/sub&gt;H&lt;sub&gt;4&lt;/sub&gt; and hexane isomers. The slim channels connecting the large cavities act as screening sites for matching-sized molecules to pass through, while the large cavities function as storage sites for large adsorption capacity. Orthogonal-array MOFs, like JNU-3a, feature one-dimensional (1D) channels that enable rapid diffusion, complemented by molecular pockets on both sides that facilitate selective recognition. The dynamic “gourd-shaped” opening of the pocket demonstrates notable adaptability when interacting with different hydrocarbons, allowing for sieving-like behavior in the separation of propylene/propane, as well as efficient separation of ethylene from its mixtures with","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 2","pages":"195–209 195–209"},"PeriodicalIF":14.0,"publicationDate":"2025-01-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143507817","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":"Pore Engineering in Metal–Organic Frameworks for Enhanced Hydrocarbon Adsorption and Separation","authors":"Xiao-Jing Xie, Min-Yi Zhou, Heng Zeng, Weigang Lu, Dan Li","doi":"10.1021/accountsmr.4c00336","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00336","url":null,"abstract":"The separation and purification of hydrocarbons are crucially important processes in the petrochemical industry, as they are essential for producing high-quality chemicals and fuels. However, traditional thermal-driven separation practices, such as cryogenic distillation, are notoriously energy-intensive, accounting for a notable portion of the energy consumption in industrial operations. This has spurred the exploration and development of low-energy and sustainable alternative separation technologies, among which adsorption/desorption-based separation with porous materials has gained significant attention. Metal–organic frameworks (MOFs) are emerging as ideal porous materials for hydrocarbon separation due to their exceptional porosity and structural tunability. This Account delves into the latest advancements in microporous MOFs for hydrocarbon separation, categorizing them based on their pore structures: single array, tandem array, and orthogonal array. Single-array MOFs feature uniformly arranged channel-like pores along the axial direction, facilitating the incorporation of binding sites on the pore surfaces. One notable functional group used in these applications is open metal sites (OMSs), which can engage in strong metal-π interactions with unsaturated hydrocarbons such as acetylene. For example, JNU-1 demonstrates increased binding energy with the increasing pressure of acetylene due to the induce-fit effect, where framework contraction behavior is triggered by its OMSs. JNU-4 offers two binding sites per metal center for acetylene molecules, greatly improving the adsorption capacity. On the other hand, introducing low-polarity groups, as seen in JNU-6-CH&lt;sub&gt;3&lt;/sub&gt;, can effectively enhance the separation performance in favor of alkanes while maintaining structural integrity under humid conditions. Another methyl group-modified MOF, JNU-5-CH&lt;sub&gt;3&lt;/sub&gt;, exhibits an acetylene-triggered gate-opening effect due to the multiple supramolecular interactions with acetylene. Tandem-array MOFs provide enhanced selectivity and adsorption capacity through the interconnection of spacious cavities with narrow apertures. For instance, JNU-2 with pore-channel interconnected structure exhibits improved separation efficiency for C&lt;sub&gt;2&lt;/sub&gt;H&lt;sub&gt;6&lt;/sub&gt;/C&lt;sub&gt;2&lt;/sub&gt;H&lt;sub&gt;4&lt;/sub&gt; and hexane isomers. The slim channels connecting the large cavities act as screening sites for matching-sized molecules to pass through, while the large cavities function as storage sites for large adsorption capacity. Orthogonal-array MOFs, like JNU-3a, feature one-dimensional (1D) channels that enable rapid diffusion, complemented by molecular pockets on both sides that facilitate selective recognition. The dynamic “gourd-shaped” opening of the pocket demonstrates notable adaptability when interacting with different hydrocarbons, allowing for sieving-like behavior in the separation of propylene/propane, as well as efficient separation of ethylene from its mixtures with alk","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"22 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142935672","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":"Advanced Cathodes for Practical Lithium–Sulfur Batteries","authors":"Jang-Yeon Hwang,&nbsp;Hyeona Park,&nbsp;Hun Kim,&nbsp;Shivam Kansara and Yang-Kook Sun*,&nbsp;","doi":"10.1021/accountsmr.4c0036810.1021/accountsmr.4c00368","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00368https://doi.org/10.1021/accountsmr.4c00368","url":null,"abstract":"&lt;p &gt;Sulfur, being lightweight, cost-effective, and offering a remarkably high lithium-ion storage capacity, has positioned lithium–sulfur (Li–S) batteries as promising candidates for applications that demand high energy density. These range from electric vehicles (EVs) to urban air mobility (UAM) systems. Despite this potential, Li–S batteries still face significant performance challenges, limiting their practical application. Chief among these challenges are the limited lifespan and low charge–discharge efficiency, predominantly caused by the dissolution of lithium polysulfide intermediate products formed during battery cycling in ether-based electrolytes. Moreover, sulfur and lithium sulfide, which constitute the active material in the cathode, are intrinsically insulating, complicating efforts to increase the active material content in the cathode and fabricate thick cathodes with high conductivity. These issues have long stood in the way of Li–S batteries achieving commercial viability. Overcoming these obstacles requires a multifaceted approach that focuses on modifications at the level of the cathode materials such as the active material, conductive agents, binders, and additives. This Account delves into these key challenges and presents a comprehensive overview of research strategies aimed at enhancing the performance of Li–S batteries with a particular focus on the sulfur cathode. First, the Account addresses practical challenges in Li–S batteries, such as the complex composition of the cathode, the low sulfur utilization efficiency, suboptimal electrolyte-to-sulfur ratios, and nonuniform sulfur conversion reactions. Strategies to overcome these barriers include the design of advanced cathode architectures that promote high sulfur utilization and an improved energy density. Modifications to the components of the cathode and the adjoining materials, such as the incorporation of conductive additives, help mitigate the insulating nature of sulfur.&lt;/p&gt;&lt;p &gt;Additionally, the Account places particular emphasis on the innovative use of pelletizing techniques in sulfur cathode fabrication, which has demonstrated notable improvements in the cathode performance. One of the Account’s highlights is the discussion of low-temperature operation strategies for Li–S batteries, which is a critical area for real-world application, especially in aerospace and cold-environment operations. There are significant performance differences when transitioning from lab-scale coin cells to larger pouch cells, underscoring the importance of considering cell geometries and their impact on the scalability and performance. Finally, the Account explores the development of all-solid-state Li–S batteries, a promising approach that could fundamentally address the issue of lithium polysulfide dissolution by eliminating the use of liquid electrolytes altogether. The inherent drawbacks of Li–S batteries, such as the insulating nature of sulfur and the challenges of high sulfur ","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"6 2","pages":"245–258 245–258"},"PeriodicalIF":14.0,"publicationDate":"2025-01-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143507816","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":"Advanced Cathodes for Practical Lithium–Sulfur Batteries","authors":"Jang-Yeon Hwang, Hyeona Park, Hun Kim, Shivam Kansara, Yang-Kook Sun","doi":"10.1021/accountsmr.4c00368","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00368","url":null,"abstract":"Sulfur, being lightweight, cost-effective, and offering a remarkably high lithium-ion storage capacity, has positioned lithium–sulfur (Li–S) batteries as promising candidates for applications that demand high energy density. These range from electric vehicles (EVs) to urban air mobility (UAM) systems. Despite this potential, Li–S batteries still face significant performance challenges, limiting their practical application. Chief among these challenges are the limited lifespan and low charge–discharge efficiency, predominantly caused by the dissolution of lithium polysulfide intermediate products formed during battery cycling in ether-based electrolytes. Moreover, sulfur and lithium sulfide, which constitute the active material in the cathode, are intrinsically insulating, complicating efforts to increase the active material content in the cathode and fabricate thick cathodes with high conductivity. These issues have long stood in the way of Li–S batteries achieving commercial viability. Overcoming these obstacles requires a multifaceted approach that focuses on modifications at the level of the cathode materials such as the active material, conductive agents, binders, and additives. This Account delves into these key challenges and presents a comprehensive overview of research strategies aimed at enhancing the performance of Li–S batteries with a particular focus on the sulfur cathode. First, the Account addresses practical challenges in Li–S batteries, such as the complex composition of the cathode, the low sulfur utilization efficiency, suboptimal electrolyte-to-sulfur ratios, and nonuniform sulfur conversion reactions. Strategies to overcome these barriers include the design of advanced cathode architectures that promote high sulfur utilization and an improved energy density. Modifications to the components of the cathode and the adjoining materials, such as the incorporation of conductive additives, help mitigate the insulating nature of sulfur.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"28 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142935077","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}