Angewandte Chemie最新文献_第7页

Photoelektrochemie individueller Al:SrTiO3/Rh2−yCryO3 Photokatalysator Partikel für Wasserstoff- und Sauerstoffentwicklung 单体铝：SrTiO3/Rh2−yCryO3光催化剂用于氢和氧发展的颗粒

Angewandte Chemie Pub Date : 2025-08-25 DOI: 10.1002/ange.202516520

Gaukhar Askarova, Dr. Chengcan Xiao, Shu Wu, Kim Kisslinger, Prof. Frank E. Osterloh, Prof. Michael V. Mirkin

引用次数: 0

Lattice-Engineered Lanthanide Nanocrystals with Tunable Near-Infrared-IIb Lifetime 具有可调近红外寿命的晶格工程镧系纳米晶体

Angewandte Chemie Pub Date : 2025-08-25 DOI: 10.1002/ange.202513988

Dr. Feng Ren, Feng Wu, Dr. Sisi Ling, Dr. Yejun Zhang, Prof. Chunyan Li, Prof. Jiang Jiang, Dr. Hongchao Yang, Prof. Qiangbin Wang

引用次数: 0

Mechanochemical Degradation of Polystyrene Into Benzene for Recycling and Upcycling 聚苯乙烯的机械化学降解成苯的回收和升级利用

Angewandte Chemie Pub Date : 2025-08-25 DOI: 10.1002/ange.202512687

Ming-Chi Wang, Junyang Li, Ashley Zelina, Benjamin Pepper, Prof.Dr. Junpeng Wang

{"title":"Mechanochemical Degradation of Polystyrene Into Benzene for Recycling and Upcycling","authors":"Ming-Chi Wang, Junyang Li, Ashley Zelina, Benjamin Pepper, Prof.Dr. Junpeng Wang","doi":"10.1002/ange.202512687","DOIUrl":"https://doi.org/10.1002/ange.202512687","url":null,"abstract":"Synthetic plastics sourced from petroleum have gained widespread use since the 1950s. Polystyrene (PS) is one of the most extensively used plastics, as it is colorless, has high mechanical strength, and exhibits excellent chemical and thermal stability; however, it is also one of the least recycled plastics because of the high cost and low profit in recycling. Herein, we demonstrate a mechanochemical recycling approach that allows PS to be efficiently degraded into benzene when it is ground in a ball mill with AlCl3. For example, when 165 kDa PS pellets are milled with AlCl3, the extent of degradation reaches 90% at 15 min. Isotope labeling experiments indicate that both ambient water and the polymer backbone can be proton sources for the formation of benzene. The benzene generated in the mechanochemical degradation can be used to synthesize styrene, which can be repolymerized to produce polystyrene, allowing for the closed-loop recycling of PS. In addition, a mechanochemical Friedel–Crafts acylation between the generated benzene and the subsequently added benzoic anhydride produces benzophenone in 40%–50% yield. The mechanochemical degradation process demonstrated here is solvent-free, cost-effective, and energy-efficient, providing a promising route for the chemical recycling and upcycling of PS.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 41","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-08-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202512687","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145230841","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

A Self-Assembled Protein Platform for Plug-and-Play Customization of Multivalent Artificial Antibodies and Antibody-Drug Conjugates 多价人工抗体和抗体-药物偶联物的即插即用定制自组装蛋白质平台

Angewandte Chemie Pub Date : 2025-08-25 DOI: 10.1002/ange.202506426

Yuzhe Chen, Yunchuan Huang, Shisheng Wang, Xinyuan Wang, Hongyu Lu, Jie Chen, Jing Li, Zhuo Chen, Zhao Li, Tianshan She, Youmei Jin, Yuanping Gao, Jie Zhang, Lijun Wang, Wenjuan Zeng, Hong Zhu, Ze Tao, Prof. Xiaofeng Lu, Prof. Hao Yang

{"title":"A Self-Assembled Protein Platform for Plug-and-Play Customization of Multivalent Artificial Antibodies and Antibody-Drug Conjugates","authors":"Yuzhe Chen, Yunchuan Huang, Shisheng Wang, Xinyuan Wang, Hongyu Lu, Jie Chen, Jing Li, Zhuo Chen, Zhao Li, Tianshan She, Youmei Jin, Yuanping Gao, Jie Zhang, Lijun Wang, Wenjuan Zeng, Hong Zhu, Ze Tao, Prof. Xiaofeng Lu, Prof. Hao Yang","doi":"10.1002/ange.202506426","DOIUrl":"https://doi.org/10.1002/ange.202506426","url":null,"abstract":"Modular assembly of multivalent therapeutics with precise modulation of pharmacokinetic and pharmacological properties remains a critical challenge in drug development. Here, we present ATPlug, a self-assembling protein platform that integrates three crucial functional modules: a trimerization domain to enhance avidity, a SpyCatcher module for efficient conjugation, and an albumin-binding domain to optimize pharmacokinetics and tissue selectivity. This rational design facilitates the modular assembly of multivalent artificial antibodies and antibody-drug conjugates (ADCs), demonstrating remarkable versatility through the successful incorporation of diverse therapeutic modules targeting epidermal growth factor receptor (EGFR), programmed cell death ligand 1 (PD-L1), and vascular endothelial growth factor (VEGF). The trivalent constructs exhibited up to 30-fold enhancement in target binding avidity and extended plasma half-life via endogenous albumin hitchhiking. Notably, the ATPlug-customized modular ADCs achieved binding affinities of 1.8 nM for EGFR and exhibited selective cytotoxicity toward EGFR-overexpressing tumor cells, resulting in potent tumor suppression efficacy. This plug-and-play strategy provides a framework for next-generation therapeutics combining customized multivalency with multidrug synergies.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 40","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-08-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145172024","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

Boosting Nitrate-to-Ammonia Conversion over Copper-Based Electrocatalysts by Facilitating Hydrogenation and Product Desorption 铜基电催化剂促进加氢和产物脱附，促进硝酸盐转化为氨

Angewandte Chemie Pub Date : 2025-08-25 DOI: 10.1002/ange.202509090

Yunying Wang, Tong Bao, Liyan Chen, Chaoqi Zhang, Jing Wang, Yingying Zou, Yamin Xi, Zhijie Li, Prof. Chengzhong Yu, Prof. Chao Liu

{"title":"Boosting Nitrate-to-Ammonia Conversion over Copper-Based Electrocatalysts by Facilitating Hydrogenation and Product Desorption","authors":"Yunying Wang, Tong Bao, Liyan Chen, Chaoqi Zhang, Jing Wang, Yingying Zou, Yamin Xi, Zhijie Li, Prof. Chengzhong Yu, Prof. Chao Liu","doi":"10.1002/ange.202509090","DOIUrl":"https://doi.org/10.1002/ange.202509090","url":null,"abstract":"Electrocatalytic nitrate reduction reaction (NitRR) in neutral condition offers a sustainable route for ammonia (NH3) production and water purification. For the most extensively investigated Cu-based electrocatalysts that favor NO3− adsorption, insufficient hydrogenation capability and sluggish NH3 desorption hinder the ultimate performance. Herein, we report Ca-doped Cu2O co-modified by oxalate (Ca─Cu2O─OA) as a novel and high-performance NitRR electrocatalyst. Experimental and theoretical results demonstrate that the Ca dopant with strong hydration effect facilitates the hydrogenation steps of adsorbed NO3− on the adjacent Cu active sites. The hydrogen-bonding interaction between OA and adsorbed NH3 promotes the product desorption. Together with the strong NO3− adsorption capability and inhibited hydrogen evolution as a side reaction, excellent NitRR performance with a high Faraday efficiency (FE) of 97.49% and a high NH3 yield of 15.02 mg h−1 cm−2 is achieved in neutral condition, outperforming most reported electrocatalysts. This work has provided new insights into the rational design of advanced NitRR electrocatalysts.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 41","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-08-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145230812","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

Frontispiece: Merging Photocatalysis with Chiral Lewis Acid Catalysis for Enantioselective Hydrosilylation/Hydrogermylation of Electron-Deficient Alkenes 前言：光催化与手性路易斯酸催化在缺电子烯烃对映选择性硅氢化/氢基化中的融合

Angewandte Chemie Pub Date : 2025-08-25 DOI: 10.1002/ange.202583501

引用次数: 0

Volcano-Shaped Relationship Between Interfacial K+-H2O Ratio and CO2 Reduction Activity in Tandem Electrocatalysts 串联电催化剂界面K+-H2O比与CO2还原活性的火山型关系

Angewandte Chemie Pub Date : 2025-08-25 DOI: 10.1002/ange.202514557

Prof. Lu-Hua Zhang, Yaohua Hong, Yabo Guo, Yishan Xu, Yida Du, Prof. Fei Li, Prof. Fengshou Yu

{"title":"Volcano-Shaped Relationship Between Interfacial K+-H2O Ratio and CO2 Reduction Activity in Tandem Electrocatalysts","authors":"Prof. Lu-Hua Zhang, Yaohua Hong, Yabo Guo, Yishan Xu, Yida Du, Prof. Fei Li, Prof. Fengshou Yu","doi":"10.1002/ange.202514557","DOIUrl":"https://doi.org/10.1002/ange.202514557","url":null,"abstract":"Modulating surface-active hydrogen (*H) supply represents a critical strategy to boost the electrocatalytic CO2 reduction reaction (ECRR), yet the mechanistic interplay between *H dynamics and catalytic behavior remains ambiguous. Herein, we construct tandem catalysts (M4/Ni1NC, M = Fe, Co, Cu, or Mn) by coupling tetranuclear metal clusters (M4) with single-atom Ni sites on N-doped carbon (Ni1NC) to regulate *H supply. Experimental and theoretical results reveal that the *H supply is governed by both thermodynamics and kinetic factors. The M4 clusters provide the thermodynamic feasibility for *H supply for CO2 activation. The *H supply rate in kinetic perspective is tuned by the K+-H2O ratio of interfacial water, determined by work function of the decorated M4 clusters. The increased K+-H2O ratio can promote water dissociation to maintain optimal *H coverage for intermediate hydrogenation, whereas excessive *H accumulation triggers competitive hydrogen evolution. Therefore, a volcanic relationship was observed between the K+-H2O ratio and ECRR performance. Among these samples, Cu4/Ni1NC with moderate *H supply rate in kinetic exhibits exceptional ECRR performance, achieving >95% Faradaic efficiency for CO across a 0.8 V potential range (−0.2 to −1.0 V versus RHE) and industrial-relevant current densities (∼385 mA cm−2 at −1.0 V) in a flow cell.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 41","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-08-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145230574","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

Bidirectional Hydrogen Spillover Enables High Activity Catalysts for Rechargeable Hydrogen Batteries 双向氢外溢为可充电氢电池提供高活性催化剂

Angewandte Chemie Pub Date : 2025-08-25 DOI: 10.1002/ange.202512466

Yidi Wang, Hongxu Liu, Zhenshan Lv, Dr. Yameng Fan, Dr. Guili Zhao, Jingwen Xu, Shunxin Tan, Peiyan Tong, Shuyang Wei, Ziwei Zhang, Dongyang Shen, Prof. Xiangyang Li, Dr. Taoli Jiang, Prof. Wei Chen

{"title":"Bidirectional Hydrogen Spillover Enables High Activity Catalysts for Rechargeable Hydrogen Batteries","authors":"Yidi Wang, Hongxu Liu, Zhenshan Lv, Dr. Yameng Fan, Dr. Guili Zhao, Jingwen Xu, Shunxin Tan, Peiyan Tong, Shuyang Wei, Ziwei Zhang, Dongyang Shen, Prof. Xiangyang Li, Dr. Taoli Jiang, Prof. Wei Chen","doi":"10.1002/ange.202512466","DOIUrl":"https://doi.org/10.1002/ange.202512466","url":null,"abstract":"Rechargeable hydrogen batteries exhibit superior electrochemical activity for hydrogen evolution and oxidation reactions (HER/HOR) in acidic media compared to alkaline counterparts, making them promising for large-scale energy storage. However, the development of efficient electrocatalysts for both HER and HOR in acidic media remains challenging, as conventional platinum-based catalysts face intrinsic limitations in simultaneously achieving high activity and long-term stability under harsh operating conditions. Herein, we introduce a bidirectional hydrogen spillover strategy to enable synergistic bifunctional HER/HOR catalysts for hydrogen batteries. We demonstrate a Ru–WO3 catalyst grown on Cu foam (Ru–WO3@CF), where the interaction between Ru and WO3 enables dynamic shuttling of adsorbed hydrogen species under alternating potentials. The Ru–WO3@CF electrode demonstrates exceptional HER/HOR bifunctionality in acidic media (0.5 M H2SO4), achieving an ultralow HER overpotential of 17 mV at 10 mA cm−2 and an HOR current density of 21.5 mA cm−2 at 50 mV — both significantly outperforming commercial Pt/C benchmarks. The hydrogen battery fabricated with Ru–WO3@CF demonstrates exceptional performance across a wide range of temperatures. This work aims to explore the feasibility of bidirectional hydrogen spillover in enhancing the bifunctional catalytic activities toward HER/HOR, providing new insights for high-performance hydrogen batteries.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 41","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-08-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145230813","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

Near-Full-Spectrum Emission Control in Copper(I) Iodides via Inorganic Structural Engineering Within a Single-Cation Host 基于无机结构工程的单阳离子主体内碘化铜的近全光谱发射控制

Angewandte Chemie Pub Date : 2025-08-25 DOI: 10.1002/ange.202514416

Yongjing Deng, Yongkang Zhu, Xiaodong Zhao, Ning Ding, Yong Yang, Mengzhu Wang, Jiangang Li, Prof. Pengfei She, Prof. Shujuan Liu, Prof. Yun Ma, Prof. Qiang Zhao

{"title":"Near-Full-Spectrum Emission Control in Copper(I) Iodides via Inorganic Structural Engineering Within a Single-Cation Host","authors":"Yongjing Deng, Yongkang Zhu, Xiaodong Zhao, Ning Ding, Yong Yang, Mengzhu Wang, Jiangang Li, Prof. Pengfei She, Prof. Shujuan Liu, Prof. Yun Ma, Prof. Qiang Zhao","doi":"10.1002/ange.202514416","DOIUrl":"https://doi.org/10.1002/ange.202514416","url":null,"abstract":"Hybrid copper(I) halides have emerged as a new class of optoelectronic materials due to their tunable structure and photophysical properties. However, systematically correlating inorganic polyhedra configurations with emission characteristics remains challenging. Herein, we address this by synthesizing a homologous series of copper(I) iodides templated solely by the [C13H24N]+ cation. Precise control reaction conditions yielded distinct inorganic polyhedral configurations, monomeric [CuI3]2− (1), dimeric [Cu2I4]2− (2), trimeric [Cu3I6]3− (3), and tetrameric [Cu4I6]2− (4). We establish a direct correlation where increasing inorganic aggregation systematically reduces the bandgap and dictates the luminescence color across a near-full visible spectrum, from blue (1) to cyan (2), red (3), and yellow (4). Detailed spectroscopic and theoretical analyses reveal the self-trapped excitons emission mechanism dependent on the Cu-I configuration, in which the closed [Cu4I6]2− configuration is more resistant to excited lattice deformation, thereby resulting in a lowest Stokes shift energy. Furthermore, stimuli-responsive sequential phase transitions between these well-defined structures were demonstrated, offering insights into their structural dynamics. This work provides critical fundamental understanding of how inorganic framework engineering within a fixed organic host precisely controls both electronic structure and excited-state relaxation pathways in hybrid copper(I) halides, paving the way for rational design of materials with tailored optical properties.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 41","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-08-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145230844","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 Photoresponsive Hybrid of Viruses and Supramolecular Peptide Fibers for Multidimensional Control of Patterning and Infection 病毒与超分子肽纤维的光敏杂交，用于多角度控制图案和感染

Angewandte Chemie Pub Date : 2025-08-24 DOI: 10.1002/ange.202508528

Dr. Atsuya Yaguchi, Prof. Noriyuki Uchida, Daiki Miura, Prof. Go Watanabe, Prof. Hirotsugu Hiramatsu, Prof. Itsuki Ajioka, Prof. Teruhiko Matsubara, Prof. Toshinori Sato, Chinbat Enkhzaya, Shunto Itani, Tomokazu Saito, Prof. Takahiro Muraoka

{"title":"A Photoresponsive Hybrid of Viruses and Supramolecular Peptide Fibers for Multidimensional Control of Patterning and Infection","authors":"Dr. Atsuya Yaguchi, Prof. Noriyuki Uchida, Daiki Miura, Prof. Go Watanabe, Prof. Hirotsugu Hiramatsu, Prof. Itsuki Ajioka, Prof. Teruhiko Matsubara, Prof. Toshinori Sato, Chinbat Enkhzaya, Shunto Itani, Tomokazu Saito, Prof. Takahiro Muraoka","doi":"10.1002/ange.202508528","DOIUrl":"https://doi.org/10.1002/ange.202508528","url":null,"abstract":"Viruses are versatile colloidal materials in their biofunctions, monodispersed and periodic structures, and high surface designability. For expanding the applicability of virus-based materials, spatiotemporally controlled immobilization and dispersion of viruses with retained activity should be useful, though control of the dynamic nature of viruses hybridized with commonly used polymers has been difficult due to their strong interactions. Here, we report a self-assembling peptide (A2Az) enabling photo control of adhesion and dispersion of M13 bacteriophage virus (M13 phage) and successfully demonstrate patterning of localization and infection of the virus. A2Az is a cationic peptide with amphiphilicity that consists of eight amino acid residues containing a photo-responsive azobenzene group at the second position and self-assembles into a helical supramolecular fiber to form a hydrogel. The helical fibrillar morphology of A2Az exhibits strong interaction with M13 phage, allowing for immobilization not only on a two-dimensional surface but also in a three-dimensional hydrogel with suppression of infectivity. The A2Az fiber undergoes a light-triggered fiber-to-particle transition and releases the immobilized M13 phage with retained infectivity for the photo-controlled patterning of localization and infection. This approach has potential applicability to various virus-based biomaterials, such as structural materials and materials for photo-selective gene transfection to cells.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 41","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-08-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202508528","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145230725","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