Angewandte Chemie最新文献

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Asymmetric Radical Coupling to Form β2,2,3-Amino Acid Esters by Synergistic Chiral Phosphoric Acid and Photocatalysis 手性磷酸与光催化作用下不对称自由基偶联生成β2,2,3-氨基酸酯
Angewandte Chemie Pub Date : 2025-08-23 DOI: 10.1002/ange.202514155
Zi-Wei He, Bao-Ru Yuan, Prof. Xiao-Ye Yu, Min Jiang, Prof. Jia-Rong Chen, Prof. Wen-Jing Xiao
{"title":"Asymmetric Radical Coupling to Form β2,2,3-Amino Acid Esters by Synergistic Chiral Phosphoric Acid and Photocatalysis","authors":"Zi-Wei He,&nbsp;Bao-Ru Yuan,&nbsp;Prof. Xiao-Ye Yu,&nbsp;Min Jiang,&nbsp;Prof. Jia-Rong Chen,&nbsp;Prof. Wen-Jing Xiao","doi":"10.1002/ange.202514155","DOIUrl":"https://doi.org/10.1002/ange.202514155","url":null,"abstract":"<p>β-Amino acids are essential building blocks in bioactive molecules, offering unique properties and potential in peptide and drug synthesis. Among them, β<sup>2,2,3</sup>-amino acids—characterized by a contiguous quaternary and tertiary stereocenter—represent a structurally unique subclass with promising biological potential. However, their broader application has been hampered by the scarcity of general and efficient synthetic methods. To address these challenges, we have developed a visible-light-driven radical-radical coupling strategy enabled by chiral phosphoric acid (CPA) catalysis. In this synergistic dual catalytic system, β-keto esters are activated by CPA and undergo single-electron oxidation to generate tertiary carbon radicals, while redox-active NHPI esters derived from α-amino acids are reduced via SET to form α-amino alkyl radicals. Under the chiral environment provided by CPA, these radicals engage in highly selective cross-coupling to afford β<sup>2,2,3</sup>-amino esters in good yields with excellent diastereo- and enantioselectivity. This strategy provides a mild, modular approach for the stereo-controlled assembly of structurally complex β<sup>2,2,3</sup>-amino esters, overcoming long-standing limitations in substrate scope and reaction efficiency. Beyond its synthetic utility, this method offers new opportunities for expanding the chemical space of β-amino acid derivatives and holds promise for advancing medicinal chemistry and peptide-based drug discovery.</p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 40","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-08-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145172012","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}
引用次数: 0
Stabile ultramikroporöse Metall-organische Gerüstverbindungen mit hydrophilen und hydrophoben Porenbereichen für die selektive Gasadsorption 稳定的超微孔金属有机支架,具有亲水和疏水孔隙区域,用于选择性气体吸附
Angewandte Chemie Pub Date : 2025-08-23 DOI: 10.1002/ange.202513788
Robert Oestreich, Marcus N. A. Fetzer, Yifei Zhang, Andreas Schreiber, Alexander Knebel, Markus Suta, Christoph Janiak, Gabriel Hanna, Gündoğ Yücesan
{"title":"Stabile ultramikroporöse Metall-organische Gerüstverbindungen mit hydrophilen und hydrophoben Porenbereichen für die selektive Gasadsorption","authors":"Robert Oestreich,&nbsp;Marcus N. A. Fetzer,&nbsp;Yifei Zhang,&nbsp;Andreas Schreiber,&nbsp;Alexander Knebel,&nbsp;Markus Suta,&nbsp;Christoph Janiak,&nbsp;Gabriel Hanna,&nbsp;Gündoğ Yücesan","doi":"10.1002/ange.202513788","DOIUrl":"https://doi.org/10.1002/ange.202513788","url":null,"abstract":"<p>Die ultramikroporösen Poren von TUB41 beherbergen selektiv Wasser- und CO<sub>2</sub>-Moleküle in unterschiedlichen hydrophilen und hydrophoben Bereichen, ohne dabei in Konkurrenz zu treten.\u0000\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure></p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 40","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-08-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202513788","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145172013","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Min-Jae Choi Min-Jae崔
Angewandte Chemie Pub Date : 2025-08-23 DOI: 10.1002/ange.202517869
Min-Jae Choi
{"title":"Min-Jae Choi","authors":"Min-Jae Choi","doi":"10.1002/ange.202517869","DOIUrl":"https://doi.org/10.1002/ange.202517869","url":null,"abstract":"<p>“<i>The most important future applications of my research are quantum dot sensors for autonomous vehicles and robotics… The most rewarding aspect of refereeing is helping great science become clearer and more impactful</i>…”</p><p>Find out more about Min-Jae Choi in his Introducing… Profile.\u0000\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure></p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 41","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-08-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202517869","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145230789","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
In Situ Click Chemistry Screen Facilitated by an On-Nanoparticle DNA-Encoded Library Identifies Highly Selective and Potent Peptoid Ligands for a Phosphatase 由纳米颗粒dna编码文库促进的原位点击化学筛选鉴定磷酸酶的高选择性和有效的肽类配体
Angewandte Chemie Pub Date : 2025-08-23 DOI: 10.1002/ange.202511606
Minkyung Kim, Jungyeon Kim, Hee Myeong Wang, Hyemin Kim, Dohee Ahn, Jeongsik Lee, Chang Yun Son, Sang Jeon Chung, Min Hyeon Shin, Hyun-Suk Lim
{"title":"In Situ Click Chemistry Screen Facilitated by an On-Nanoparticle DNA-Encoded Library Identifies Highly Selective and Potent Peptoid Ligands for a Phosphatase","authors":"Minkyung Kim,&nbsp;Jungyeon Kim,&nbsp;Hee Myeong Wang,&nbsp;Hyemin Kim,&nbsp;Dohee Ahn,&nbsp;Jeongsik Lee,&nbsp;Chang Yun Son,&nbsp;Sang Jeon Chung,&nbsp;Min Hyeon Shin,&nbsp;Hyun-Suk Lim","doi":"10.1002/ange.202511606","DOIUrl":"https://doi.org/10.1002/ange.202511606","url":null,"abstract":"<p>Capture agents that selectively bind to biological targets are indispensable tools in diagnostics, therapeutics, and biomedical research. However, discovering such capture agents, particularly for structurally conserved or challenging targets, remains a challenge. Here, we describe a protein-templated in situ click strategy enabled by a nanoparticle-based DNA-encoded library (nanoDEL) platform. The nanoDEL enables the construction and screening of vastly large, chemically diverse combinatorial libraries with high redundancy, far exceeding the scale and throughput of conventional approaches, such as one-bead-one-compound and solution-phase in situ click methods. Thus, this enables the rapid and efficient identification of high-affinity, high-selectivity ligands in a single selection round, eliminating the need for iterative screening. To demonstrate the utility of this strategy, we performed an in situ click screening of a 27-million-member nanoDEL of azido-functionalized peptoids, in the presence of a weak and promiscuous alkyne-bearing anchor ligand. This yielded bidentate inhibitors of protein tyrosine phosphatase 1B, a challenging target due to its highly conserved active site. These inhibitors exhibited nanomolar potency and exceptional selectivity over closely related phosphatases. This work represents a broadly applicable strategy for discovering high-performance capture agents, particularly for selectively targeting closely related protein families or isoforms where achieving selectivity remains a critical challenge.</p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 41","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-08-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145230790","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}
引用次数: 0
A Modular Three-Component Asymmetric Tsuji–Trost Reaction Enabled by Cooperative Palladium/Lewis Acid Catalysis 钯/Lewis酸协同催化的模块化三组分不对称Tsuji-Trost反应
Angewandte Chemie Pub Date : 2025-08-23 DOI: 10.1002/ange.202512977
Jun Zhang, Prof. Dr. Can Zhu
{"title":"A Modular Three-Component Asymmetric Tsuji–Trost Reaction Enabled by Cooperative Palladium/Lewis Acid Catalysis","authors":"Jun Zhang,&nbsp;Prof. Dr. Can Zhu","doi":"10.1002/ange.202512977","DOIUrl":"https://doi.org/10.1002/ange.202512977","url":null,"abstract":"<p>Asymmetric allylic substitution (AAS) reactions, named as the Tsuji–Trost reaction, stand as a landmark in modern organic synthesis. The merge of AAS reactions with the concept of multicomponent modular synthesis could allow flexible customization of molecular architectures from fundamental feedstocks, which remains underdeveloped. Herein, we disclose our recent observations on a novel three-component asymmetric Tsuji–Trost reaction enabled by cooperative palladium/Lewis acid (LA) catalysis. This ‘<i>1C</i> + <i>2C</i> + NuH’ approach starts from fundamental organic feedstocks, i.e., aldehyde, allylboronate, and a nucleophile with the in situ formation of a C═C double bond. Diverse nucleophiles have been demonstrated to be applicable in this three-component AAS reaction, including malonates, acetylacetone, acetoacetate, phosphine oxides, sulfonyl hydrazides etc. The protocol successfully offers a novel platform to integrate two distinct bioactive molecular scaffolds to access diverse array of hybrids. Mechanistic studies suggest that the three-component AAS approach proceeds via a reaction sequence of LA-catalyzed allylation of aldehyde, olefin shift under palladium catalysis, and Pd/LA-cocatalyzed asymmetric allylic substitution.</p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 41","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-08-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145230793","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}
引用次数: 0
Evolving Data-Driven Strategies for the Characterization of Supramolecular Polymers and Systems 不断发展的数据驱动策略表征超分子聚合物和系统
Angewandte Chemie Pub Date : 2025-08-22 DOI: 10.1002/ange.202509122
Stef A. H. Jansen, Ghislaine Vantomme, E. W. Meijer
{"title":"Evolving Data-Driven Strategies for the Characterization of Supramolecular Polymers and Systems","authors":"Stef A. H. Jansen,&nbsp;Ghislaine Vantomme,&nbsp;E. W. Meijer","doi":"10.1002/ange.202509122","DOIUrl":"https://doi.org/10.1002/ange.202509122","url":null,"abstract":"<p>Inspired by the dynamic assembly of fibrillar proteins in biology, research on supramolecular polymers has progressed rapidly toward the development of synthetic multicomponent systems. In this review, we highlight recent advances in the study of supramolecular polymers in solution, with an emphasis on how combined computational and experimental approaches deepen our understanding of these systems. In particular, these studies have elucidated the mechanisms of protein aggregation and provided insights into the characteristics of synthetic systems. We discuss the classification of these polymers and systems, highlighting how their different interaction modes and microstructures give rise to diverse structural and functional properties. In addition, we outline the emerging role of machine learning as a powerful tool to navigate the inherent complexity of these systems, thereby enhancing strategies for rational design and characterization. This review highlights how computational approaches, from traditional modeling to emerging machine learning techniques, enable the experimental characterization and understanding of supramolecular polymer chemistry.</p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 38","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-08-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202509122","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145062411","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Charge-Rearrangement Averaged Dye Design for Precise, Real-Time, and Portable Monitoring of Complex Solvent Environments 电荷重排平均染料设计精确,实时,便携式监测复杂的溶剂环境
Angewandte Chemie Pub Date : 2025-08-22 DOI: 10.1002/ange.202513349
Zhongyu Li, Dr. Smruti R. Sahoo, Dr. Shen Shen, Dr. Hao Sun, Prof. Hans Ågren, Dr. Man Zhang, Prof. Gleb Baryshnikov, Prof. Liangliang Zhu
{"title":"Charge-Rearrangement Averaged Dye Design for Precise, Real-Time, and Portable Monitoring of Complex Solvent Environments","authors":"Zhongyu Li,&nbsp;Dr. Smruti R. Sahoo,&nbsp;Dr. Shen Shen,&nbsp;Dr. Hao Sun,&nbsp;Prof. Hans Ågren,&nbsp;Dr. Man Zhang,&nbsp;Prof. Gleb Baryshnikov,&nbsp;Prof. Liangliang Zhu","doi":"10.1002/ange.202513349","DOIUrl":"https://doi.org/10.1002/ange.202513349","url":null,"abstract":"<p>Although solvatochromic materials provide visual function to differentiate solvents, they fail to precisely monitor complex solvent environments where solvent composition varies dynamically, because of an insensitive absorptional shift in these environments. Relatively, their fluorescence signal change, which should be more sensitive, has always been inefficient, resulting from inherent challenges in excited-state dynamics. Here, we present a charge-rearrangement averaged dye design, instead of traditional donor-acceptor structures, to enable a high locally excited or twisted intramolecular charge transfer emission efficiency. A ratiometric dual-fluorescence behavior can be observed along with a solvent-dependent emission trade-off rather than complete quenching. In this case, the dyes can not only precisely visualize various mixed solvents but also enable heterogeneous detection with over hundreds of reuse cycles after being integrated into a crosslinked polymer. The leading portable material achieves a self-calibrated visual tracking of ethanol content (error&lt;0.2%) with a robust working curve (<i>R</i><sup>2</sup> = 0.9992) while applied to E10 ethanol gasoline, operable via user-friendly software analysis through mobile phone photography.</p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 40","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-08-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145172004","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}
引用次数: 0
A Photon-Driven Unimolecular Immunostimulant for Self-Amplified Pyroptosis and cGAS-STING Pathway by Destroying the Pyroptosis Checkpoint 一种光子驱动的单分子免疫刺激剂,通过破坏焦亡检查点来促进自扩增焦亡和cGAS-STING途径
Angewandte Chemie Pub Date : 2025-08-22 DOI: 10.1002/ange.202513815
Shuang Zeng, Chen Chen, Zhihan Guo, Chunfang Qin, Yang Wang, Xiaosheng Liu, Xin Li, Hyunsun Jeong, Yifu Hao, Danhong Zhou, Prof. Saran Long, Prof. Zhenyong Wu, Prof. Jingyun Wang, Prof. Haidong Li, Prof. Xiaojun Peng, Prof. Juyoung Yoon
{"title":"A Photon-Driven Unimolecular Immunostimulant for Self-Amplified Pyroptosis and cGAS-STING Pathway by Destroying the Pyroptosis Checkpoint","authors":"Shuang Zeng,&nbsp;Chen Chen,&nbsp;Zhihan Guo,&nbsp;Chunfang Qin,&nbsp;Yang Wang,&nbsp;Xiaosheng Liu,&nbsp;Xin Li,&nbsp;Hyunsun Jeong,&nbsp;Yifu Hao,&nbsp;Danhong Zhou,&nbsp;Prof. Saran Long,&nbsp;Prof. Zhenyong Wu,&nbsp;Prof. Jingyun Wang,&nbsp;Prof. Haidong Li,&nbsp;Prof. Xiaojun Peng,&nbsp;Prof. Juyoung Yoon","doi":"10.1002/ange.202513815","DOIUrl":"https://doi.org/10.1002/ange.202513815","url":null,"abstract":"<p>Immunotherapy is a groundbreaking approach for clinically treating tumors, but its effectiveness is hindered by the tumor's immunosuppressive environment and lack of immune cell infiltration, enabling tumors to evade the immune system. Although the activation of both innate and adaptive immunities is a promising strategy to counteract this bottleneck, their synergy remains challenging. Therefore, we developed <b>Bio-Cy</b>, an unprecedented organic unimolecular photosensitive immunostimulant, which stimulates self-amplifying pyroptosis and cGAS-STING pathways by disrupting pyroptosis checkpoints to enhance adaptive and innate immunity activation. Mechanistic studies have shown that <b>Bio-Cy</b> can target cancer cells and be transported to lysosomes via endocytosis, generating reactive oxygen species through a Type I photodynamic mechanism to destroy cancer cells, even under hypoxic conditions. Interestingly, this lysosomal disruption not only activates the caspase-3/GSDME-dependent pyroptosis of adaptive immunity through mitochondrial damage by releasing Ca<sup>2+</sup>, but also enhances the cGAS-STING innate immune pathway by releasing mitochondrial DNA. More importantly, the initial lysosomal damage impairs protective cellular autophagy, destroying the pyroptosis checkpoint and thus preventing the clearance of damaged mitochondria and amplifying immune responses, ultimately boosting immunotherapy. This strategy effectively treats primary tumors and inhibits metastatic growth, offering a new paradigm for photoimmunotherapy.</p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 41","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-08-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202513815","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145230649","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Bionic Design of Ni4+ Lewis Acid Site Based on Selective Seawater Oxidation 基于选择性海水氧化的Ni4+ Lewis酸位点仿生设计
Angewandte Chemie Pub Date : 2025-08-22 DOI: 10.1002/ange.202511867
Huimin Mao, Xiaobin Liu, Tong Cui, Junheng Tang, Zhi Su, Jingqi Chi, Yongming Chai, Zexing Wu, Lei Wang
{"title":"Bionic Design of Ni4+ Lewis Acid Site Based on Selective Seawater Oxidation","authors":"Huimin Mao,&nbsp;Xiaobin Liu,&nbsp;Tong Cui,&nbsp;Junheng Tang,&nbsp;Zhi Su,&nbsp;Jingqi Chi,&nbsp;Yongming Chai,&nbsp;Zexing Wu,&nbsp;Lei Wang","doi":"10.1002/ange.202511867","DOIUrl":"https://doi.org/10.1002/ange.202511867","url":null,"abstract":"<p>The side reaction caused by chloride ions and the toxicity to the active site have always been the hindrance to the electrocatalyst of the oxygen evolution reaction (OER) for seawater splitting. Herein, inspired by the early flowering of damaged plants, we designed a catalyst rich in oxygen vacancies (O<sub>vac</sub>) and proved that O<sub>vac</sub> can accelerate the formation of Ni<sup>3+</sup> and further oxidize it to Ni<sup>4+</sup>, which we named as the “ripening” mechanism of O<sub>vac</sub>. O<sub>vac</sub> reduces the hydrogen proton desorption energy by regulating local charge redistribution, thus realizing the rapid transformation of Ni<sup>2+</sup>→Ni<sup>3+</sup>→Ni<sup>4+</sup>. Meanwhile, the hard Lewis acid Ni<sup>4+</sup> has strong selectivity to OH<sup>−</sup>, avoiding the competitiveness and corrosiveness of chloride ions in seawater. This work provides an effective strategy for the simple and rapid construction of self-rebuilding high-valence Ni<sup>4+</sup> electrocatalysts, and is expected to provide guidance for the development of seawater electrolysis.</p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 41","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-08-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145230650","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}
引用次数: 0
General Synthesis of 2D Mesoporous Multimetal Spinel Supracrystals for High-Efficiency Electrochemical Applications 用于高效电化学应用的二维介孔多金属尖晶石超晶的一般合成
Angewandte Chemie Pub Date : 2025-08-22 DOI: 10.1002/ange.202510954
Yifan Gao, Shenxin Xia, Huang Fang, Zhebin Zhang, Prof. Dong Yang, Prof. Tongtao Li, Prof. Wei Li, Prof. Angang Dong
{"title":"General Synthesis of 2D Mesoporous Multimetal Spinel Supracrystals for High-Efficiency Electrochemical Applications","authors":"Yifan Gao,&nbsp;Shenxin Xia,&nbsp;Huang Fang,&nbsp;Zhebin Zhang,&nbsp;Prof. Dong Yang,&nbsp;Prof. Tongtao Li,&nbsp;Prof. Wei Li,&nbsp;Prof. Angang Dong","doi":"10.1002/ange.202510954","DOIUrl":"https://doi.org/10.1002/ange.202510954","url":null,"abstract":"<p>Two-dimensional (2D) mesoporous metal oxide crystals that integrate atomic-level single crystallinity with ordered mesoporosity represent a promising but rarely realized class of materials, particularly in multicomponent systems. Here, we report a universal strategy for synthesizing freestanding 2D mesoporous spinel supracrystals with tunable compositions, spanning from unary to multinary spinel oxide systems. This approach decouples crystalline framework formation from mesopore generation, combining emulsion-mediated, on-surface crystallization of 2D nanocrystal superlattices with thermally-induced collective nanocrystal reorientation and facet-selective epitaxial fusion. Concurrent surface reconstruction exposes {110} facets along nanocrystal edges, which define the internal surfaces of vertically aligned mesopores. As a proof of concept, 2D mesoporous FeMnCoO supracrystals are employed as functional interlayers in lithium–sulfur (Li–S) batteries. These interlayers demonstrate strong polysulfide adsorption, accelerated redox kinetics, and enhanced Li<sup>+</sup> ion transport, enabled by their multimetal-induced electronic modulation, facet-specific catalytic activity, and 2D mesoporous architecture. As a result, Li–S cells equipped with FeMnCoO-modified separators deliver exceptional electrochemical performance, even under high sulfur loading and lean electrolyte conditions. This work addresses a longstanding challenge in reconciling ordered mesoporosity with crystallographic coherence in mesoporous materials, establishing a molecularly modular approach for synthesizing 2D mesoporous spinel crystals with programmable compositions and facet-engineered functionality.</p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 41","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-08-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145230691","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}
引用次数: 0
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