Angewandte Chemie (International ed. in English)最新文献_第7页

Cationic Selenuranes - Bench-Stable Sources of Se(III) Radicals. 阳离子硒-硒（III）自由基的台架稳定源。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-16 DOI: 10.1002/anie.202513534

Kirill Zhiliaev, Boris Maryasin, Hanspeter Kählig, Marcos Gil-Sepulcre, Javier Mateos

引用次数: 0

Integration of Multiple Enzymes Within Hydrogen-Bonded Organic Frameworks for Efficient Cascade Photocatalytic CO₂-to-Methanol Conversion in Water. 多种酶在氢键有机框架内的整合，用于高效级联光催化co2在水中转化为甲醇。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-15 DOI: 10.1002/anie.202516599

Jiakang Tang, Yifei Lei, Qingxuan Tang, Shixing Lei, Qiao-Yan Qi, Zhan-Ting Li, Jia Tian

{"title":"Integration of Multiple Enzymes Within Hydrogen-Bonded Organic Frameworks for Efficient Cascade Photocatalytic CO2-to-Methanol Conversion in Water.","authors":"Jiakang Tang, Yifei Lei, Qingxuan Tang, Shixing Lei, Qiao-Yan Qi, Zhan-Ting Li, Jia Tian","doi":"10.1002/anie.202516599","DOIUrl":"https://doi.org/10.1002/anie.202516599","url":null,"abstract":"The integration of photocatalysts and enzymes within confined environments offers a promising approach to developing artificial photosynthetic systems for sustainable CO2 conversion. However, the efficient coupling of photocatalysts with multiple enzymes to enable photo-enzymatic cascade catalysis remains a significant challenge. Herein, we report the construction of hydrogen-bonded organic frameworks (HOFs) that integrate Ru-based photocatalysts with three-enzyme cascades of formate dehydrogenase (FDH), formaldehyde dehydrogenase (FaldDH), and alcohol dehydrogenase (ADH) via in situ co-assembly in water. The RuHOF exhibits exceptional nicotinamide adenine dinucleotide (NADH) photo-regeneration activity (4.5 mM h-1), while the FDH@RuHOF hybrid converts CO2 to formic acid with a turnover frequency (TOF) of 681 h-1 (238 µM h-1) over 24 h. By engineering FDH/FaldDH/ADH@RuHOF ternary systems, we achieve sustained CO2-to-methanol conversion through photo-enzymatic cascade catalysis, delivering 2.2 mM methanol production with an apparent quantum efficiency (AQY) of 5.5% (92 µM h-1) over 24 h with 85% activity retention after five catalytic cycles. This work opens a promising avenue for the development of efficient multi-enzyme cascade artificial photosynthetic systems toward steady and recyclable CO2 valorization.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202516599"},"PeriodicalIF":16.9,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145071503","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 Spin Descriptor Map Predicts NiFe₂O₄ for Efficient Electrosynthesis of Cyclohexanone Oxime. 自旋描述子图预测NiFe2O4电合成环己酮肟的效率。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-15 DOI: 10.1002/anie.202517358

Rong Yang, Jinghui Zhao, Yongmeng Wu, Ying Gao, Bin Zhang

{"title":"A Spin Descriptor Map Predicts NiFe2O4 for Efficient Electrosynthesis of Cyclohexanone Oxime.","authors":"Rong Yang, Jinghui Zhao, Yongmeng Wu, Ying Gao, Bin Zhang","doi":"10.1002/anie.202517358","DOIUrl":"https://doi.org/10.1002/anie.202517358","url":null,"abstract":"The selective hydrogenation of NO to NH2OH governs the performance of cyclohexanone oxime electrosynthesis. However, the spin state transition during the NO-to-NH2OH process, which is directly related to reaction pathways, has long been ignored. Here, we propose a spin locking mechanism via density functional theory and sure independence screening and sparsifying operator. Magnetic sites with medium spin states stabilize the *NHO intermediate by locking the spin configuration of NO to weaken *NH2OH adsorption for high selectivity. The spin magnetic moment (µS), the angle between *N-O and the catalyst (θ), and the charge state (q) are key factors, providing a screening range of the predictive metrics (µS·θ)3 and (cos θ/q). The theoretically selected NiFe2O4 delivers 70% Faradaic efficiency for cyclohexanone oxime, and weakened *NH2OH adsorption is revealed by in situ spectroscopy. This work highlights the importance of spin regulation in adjusting the selectivity of electrosynthesis.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202517358"},"PeriodicalIF":16.9,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145071518","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

Realizing High Performance Four-Electron Zinc-Iodine Batteries with Acidic Eutectic Electrolyte. 用酸性共晶电解液实现高性能四电子锌碘电池。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-15 DOI: 10.1002/anie.202515633

Yuhuan Yan, Yucong Jiao, Peiyi Wu

{"title":"Realizing High Performance Four-Electron Zinc-Iodine Batteries with Acidic Eutectic Electrolyte.","authors":"Yuhuan Yan, Yucong Jiao, Peiyi Wu","doi":"10.1002/anie.202515633","DOIUrl":"https://doi.org/10.1002/anie.202515633","url":null,"abstract":"Achieving multi-electron redox reaction via halide ions and protons is promising for Zn─I2 batteries, yet their practical application is hindered by halide ion and proton corrosion, sluggish iodine redox kinetics and poor redox reversibility. Here, a deep eutectic solvent (ZPDES) composed with concentrated ZnCl2 and H3PO4 is engineered as the electrolyte for high performance Zn-I2 batteries. The chloride atom (Cl) and active hydrogen of H3PO4 in DES form hydrogen bonds (Cl⋯H─O) to mitigate the corrosion of Cl- and protons. Therefore, while achieving four-electron transfer by Cl-, the protons in DES can accelerate redox reaction kinetics and reduce I3 - formation for improved reversibility. Moreover, the proton can promote the (002) texture formation and reduce by-products on Zn anode. As a result, the Zn─I2 battery with ZPDES delivers a high specific capacity of 576 mA h g-1 at 0.5 A g-1 after 320 cycles, and maintains a capacity retention of 100% over 20,000 cycles at 7 A g-1.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202515633"},"PeriodicalIF":16.9,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145071586","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

Aqueous Zinc-Ion Pouch Cells: From Failure Mechanisms to Practical Solutions. 水锌离子袋电池：从失效机制到实际解决方案。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-15 DOI: 10.1002/anie.202516233

Kaiyue Zhu, Weili Xie, Weishen Yang

{"title":"Aqueous Zinc-Ion Pouch Cells: From Failure Mechanisms to Practical Solutions.","authors":"Kaiyue Zhu, Weili Xie, Weishen Yang","doi":"10.1002/anie.202516233","DOIUrl":"https://doi.org/10.1002/anie.202516233","url":null,"abstract":"Aqueous zinc-ion batteries (AZIBs) have been regarded as promising candidates for stationary energy storage owing to their low cost, inherent safety, and high volumetric energy density. To fully leverage these advantages in practical applications, the pouch cell configuration offers a favorable design with compactness and lightweight packaging. Nonetheless, commercial viability remains limited by inadequate cycling stability in pouch cells, despite the extended cycle life achieved in coin cells. In this review, we emphasize the performance gap between materials-level coin cells and device-level pouch cells and elucidate the failure mechanisms in pouch-type zinc-ion batteries. These mechanisms include internal short-circuits caused by severe zinc dendrite growth under high area capacity conditions, and high polarization resulting from by-product accumulation and hydrogen evolution due to water-induced corrosion. We then comprehensively review recent progress in zinc-ion pouch cells, highlighting strategies such as artificial protective layers on the Zn anode, separator modifications, and electrolyte design. Finally, we propose a future research direction to advance and commercialize zinc-ion battery technology.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202516233"},"PeriodicalIF":16.9,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145071557","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

One-Step Silver Leaching from Manganese-Silver Ore Enabled by Hydrogen-Bonded Network Formation. 氢键网络形成促进锰银矿一步浸银

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-15 DOI: 10.1002/anie.202514318

Zhiyuan Zeng, Bin Li, Yuntao Zheng, Jiehui Hu, Peilun Li, Dianwen Liu, Shengming Xu

{"title":"One-Step Silver Leaching from Manganese-Silver Ore Enabled by Hydrogen-Bonded Network Formation.","authors":"Zhiyuan Zeng, Bin Li, Yuntao Zheng, Jiehui Hu, Peilun Li, Dianwen Liu, Shengming Xu","doi":"10.1002/anie.202514318","DOIUrl":"https://doi.org/10.1002/anie.202514318","url":null,"abstract":"Silver is an increasingly scarce resource, necessitating green leaching methods for low-grade ores. Conventional cyanidation, however, suffers from extreme toxicity and environmental hazards that make it unsustainable. We report a nontoxic synergistic leaching system based on oxalic acid and cyano-functionalized branched quaternary ammonium salts. Under mild conditions, this one-step method enables efficient and selective leaching of lattice-confined silver from polymetallic manganese-silver ore, with recoveries exceeding 90%. Kinetic studies reveal a two‑stage process, with an initial rapid dissolution of exposed manganese oxides releasing silver followed by a slower breakdown of the iron matrix to liberate encapsulated minerals. The core breakthrough is the discovery that AgCl combines with chloride anions from the quaternary ammonium salt to form a unique inorganic helical chain structure. The stability of this helical assembly is attributed to an ordered CH…Cl- H-bonded network. Spectroscopic characterization and theoretical calculations confirm that this network undergoes an energetically favorable reconstruction that overcomes the high lattice energy of AgCl. This finding demonstrates that the cooperative effect of weak H-bonds can dissociate covalently stabilized solids. Our study thus provides an innovative strategy for sustainable silver metallurgy and introduces a new paradigm of H-bond-directed metallurgical design.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202514318"},"PeriodicalIF":16.9,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145071548","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

Multi-Site Organoboron Catalysts Enable Sequence-Regulated Terpolymerization of Epoxides, CO₂, and β-Propiolactone via Intermolecular Chain Shuttling. 多位点有机硼催化剂通过分子间链穿梭实现了环氧化合物、CO2和β-丙内酯的序列调控共聚合。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-15 DOI: 10.1002/anie.202517263

Rui Yan, Ming-Jun Li, Shuai Li, Bo Li, Guang-Peng Wu

{"title":"Multi-Site Organoboron Catalysts Enable Sequence-Regulated Terpolymerization of Epoxides, CO2, and β-Propiolactone via Intermolecular Chain Shuttling.","authors":"Rui Yan, Ming-Jun Li, Shuai Li, Bo Li, Guang-Peng Wu","doi":"10.1002/anie.202517263","DOIUrl":"https://doi.org/10.1002/anie.202517263","url":null,"abstract":"Sequence regulation in synthetic polymers is essential for tailoring material properties; however, achieving precise control in polycarbonate-polyhydroxyalkanoate (PC-PHA) terpolymers derived from epoxides, CO2, and β-lactones remains challenging. Current metal-based catalysts lack multisite strategies for sequence diversification, limiting the formation of gradient architectures. This study employed mononuclear (catalyst 1) and dinuclear (catalyst 2) organoboron catalysts to mediate the terpolymerization of epoxides, CO2, and β-propiolactone (BPL). Kinetic analysis, NMR spectroscopy, and a chain-shuttling approach with mixed catalysts were utilized to regulate sequences. Key findings indicated: i) Catalyst 1 preferentially promoted β-propiolactone ring-opening polymerization (ROP), forming tapered P3HP-b-PC blocks, whereas catalyst 2 enhanced epoxide/CO2 ring-opening copolymerization (ROCOP), yielding PC-b-P3HP; ii) Boron centers kinetically suppressed ROP but increased ROCOP efficiency; iii) Mixed 1 and 2 catalysts enabled intermolecular chain shuttling, synthesizing gradient PC-grad-P3HP terpolymers; and iv) Terpolymer compositions modulated thermal properties from amorphous to crystalline. This work establishes the first metal-free, chain-shuttling platform for sequence-regulated PC-PHA terpolymers, extending the scope of programmable biodegradable materials beyond metal-catalyzed systems.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202517263"},"PeriodicalIF":16.9,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145071546","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

Hot Electron Photocatalysis Using Nontoxic Self-Doped Quantum Dots. 利用无毒自掺杂量子点进行热电子光催化。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-15 DOI: 10.1002/anie.202508543

Jianning Feng, Kezhou Fan, Qinxuan Cao, Wenfei Liang, Pui Ying Wong, Jie Xue, Kin Ting Chang, Kam Sing Wong, Haipeng Lu

{"title":"Hot Electron Photocatalysis Using Nontoxic Self-Doped Quantum Dots.","authors":"Jianning Feng, Kezhou Fan, Qinxuan Cao, Wenfei Liang, Pui Ying Wong, Jie Xue, Kin Ting Chang, Kam Sing Wong, Haipeng Lu","doi":"10.1002/anie.202508543","DOIUrl":"https://doi.org/10.1002/anie.202508543","url":null,"abstract":"Colloidal semiconductor quantum dots (QDs) have emerged as versatile photocatalysts for organic transformations. However, a significant drawback is their reliance on toxic metals like lead and cadmium, which limits their widespread application in solar-to-chemical conversion. Furthermore, current systems primarily utilize band-edge carriers for simpler photoredox reactions, while the potential for harvesting hot carriers in chemical transformations remains largely unexplored. To address these challenges, we developed nontoxic, cost-effective, and recyclable ternary CuInS2 and quaternary Cu─In─Zn─S QDs as potent photocatalysts. Our findings demonstrate that hot electrons can be effectively generated through an ultrafast Auger process, enabling the photoreduction of aryl halides (with reduction potentials up to -2.90 V versus saturated calomel electrode (SCE)) and various cross-coupling (C─C, C─P, C─B, and C─S) transformations. Notably, quaternary Cu─In─Zn─S QDs exhibit significantly higher reactivity compared to CuInS2 QDs, which is attributed to enhanced Auger-mediated hot electron generation. This work underscores the potential of directly utilizing Auger-generated hot electrons for extreme-potential organic transformations under mild conditions using nontoxic QDs.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202508543"},"PeriodicalIF":16.9,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145071520","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

Total Synthesis of Calyciphylline F. 茶碱F的全合成。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-15 DOI: 10.1002/anie.202517671

Ryota Sato, Ryuichi Sumida, Masaki Inoue, Ryota Kotaka, Sangita Karanjit, Kosuke Namba

引用次数: 0

Self-Consistent Cation-Anion Integration Eliminates Passivation Crosstalk for Inverted Perovskite Solar Cells. 自一致的正负离子集成消除了反向钙钛矿太阳能电池的钝化串扰。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-15 DOI: 10.1002/anie.202509782

Zhen Guan, Zejun Wei, Xiangyu Sun, Yihan Zhang, Zhihao Chai, Qingya Wang, Yansong Yue, Yao Zhang, Ziying Li, Mengfan Qiu, Fangze Liu, Qi Chen, Yihua Chen, Jing Wei, Hongbo Li

{"title":"Self-Consistent Cation-Anion Integration Eliminates Passivation Crosstalk for Inverted Perovskite Solar Cells.","authors":"Zhen Guan, Zejun Wei, Xiangyu Sun, Yihan Zhang, Zhihao Chai, Qingya Wang, Yansong Yue, Yao Zhang, Ziying Li, Mengfan Qiu, Fangze Liu, Qi Chen, Yihua Chen, Jing Wei, Hongbo Li","doi":"10.1002/anie.202509782","DOIUrl":"https://doi.org/10.1002/anie.202509782","url":null,"abstract":"The wide-bandgap (WBG) absorber in silicon/perovskite tandem solar cells face persistent challenges of interfacial defects and energy-level misalignment. Although dual-cation passivators have demonstrated the potential to address these issues simultaneously, their efficacy is hindered by cation competition for binding sites and modification conflicts, which limit further device improvement. To overcome these limitations, we introduce a self-consistent cation-anion integrated passivation (SCAP) strategy, designing a multifunctional passivator, PDA(TFA)2, where the bipolar trifluoroacetate (TFA) anion is paired with 1,3-propanediamine (PDA) cations. This SCAP approach eliminates cation competition by enabling defect and field-effect passivation in a unified framework. Specifically, the bipolar TFA anion efficiently passivates halide vacancies and bridges the perovskite and C60 interface, while the PDA cations induce surface dipoles and optimize band alignment. Therefore, optimized 1.68 eV WBG perovskite solar cells achieve a high power conversion efficiency (PCE) of 23.23% with an exceptional open-circuit voltage of 1.27 V. Furthermore, this strategy achieves a 32.33% PCE (31.47% certified stabilized PCE) for a 0.945 cm2 monolithic perovskite/silicon tandem cell, delivering an ultra-high 1.992 V open-circuit voltage. These findings underscore the transformative potential of the SCAP strategy in advancing the efficiency and stability of WBG perovskite photovoltaics, paving the way for next-generation tandem solar cells.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202509782"},"PeriodicalIF":16.9,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145071574","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