Angewandte Chemie (International ed. in English)最新文献

Dynamic Covalent Radical Recombination for the Assembly of Tuneable Responsive Porous Organic Cages. 可调谐响应性多孔有机笼组装的动态共价自由基重组。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2026-05-09 DOI: 10.1002/anie.7638565

Yannic Hartmann, Robert Oestreich, Yuki Wada, Philippe de Bary, Masaki Kawano, Christoph Janiak, Bernd M Schmidt

{"title":"Dynamic Covalent Radical Recombination for the Assembly of Tuneable Responsive Porous Organic Cages.","authors":"Yannic Hartmann, Robert Oestreich, Yuki Wada, Philippe de Bary, Masaki Kawano, Christoph Janiak, Bernd M Schmidt","doi":"10.1002/anie.7638565","DOIUrl":"https://doi.org/10.1002/anie.7638565","url":null,"abstract":"The construction of discrete organic cages via radical recombination offers a powerful yet underexplored route toward stimuli-responsive, C─C-linked molecular architectures. Here, we introduce aryldicyanomethyl radical dynamic covalent chemistry as a general strategy for the controlled assembly of porous organic cages. Systematic variation of a single substituent governs both radical and σ-bond stability as well as the resulting cage geometry, enabling precise, substituent-dependent control over cage topology and responsiveness. A thiophenoxy-substituted monomer S selectively affords a discrete Tri2 dimer in 99% yield, whereas the N-methylaniline-substituted analogue N forms the tetrahedral Tri4 tetramer in 83% yield. N4 possesses permanent porosity and pronounced selectivity for CO2 and H2 over CH4 and N2, as confirmed by gas sorption experiments, arising from narrow pore apertures and strong host-guest interactions. Both cages display reversible mechano- and thermochromic behaviour. Moreover, the combination of a highly dynamic bond formation process with three-dimensional preorganisation of the cage enables efficient self-healing, which is markedly accelerated upon exposure to THF vapour. Collectively, these results establish radical recombination as an unexplored dynamic covalent motif for the synthesis of responsive organic cage architectures, enabling substituent-dependent fine-tuning of topology, stability, and material function through simple substituent modification.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e7638565"},"PeriodicalIF":16.9,"publicationDate":"2026-05-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147864877","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

Hierarchical Mesoscale Trapping Controls Pathway Selection in Supramolecular Polymerization. 分级中尺度捕获控制超分子聚合的途径选择。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2026-05-09 DOI: 10.1002/anie.7258562

Ziyuan Li, Rongzhou Du, Yun Huang, Ningdong Huang, Feng Wang

{"title":"Hierarchical Mesoscale Trapping Controls Pathway Selection in Supramolecular Polymerization.","authors":"Ziyuan Li, Rongzhou Du, Yun Huang, Ningdong Huang, Feng Wang","doi":"10.1002/anie.7258562","DOIUrl":"https://doi.org/10.1002/anie.7258562","url":null,"abstract":"Supramolecular polymerization often proceeds through competing kinetic and thermodynamic pathways, giving rise to pathway complexity that governs the structure and function of supramolecular materials. While pathway selection is typically interpreted in terms of molecular packing, the potential regulatory role of organization beyond the molecular scale remains largely unexplored. Here we demonstrate that hierarchical mesoscale aggregation can control pathway selection during supramolecular polymerization. A donor-acceptor dicyanostilbene derivative forms two primary aggregates that further assemble into mesoscale structures under concentrated conditions. Time-resolved small-angle x-ray scattering combined with spectroscopy reveals that mesoscale clusters transiently trap metastable assemblies, thereby delaying their conversion into thermodynamically favored fibers. Increasing temperature enables escape from this mesoscale trap, directly switching the assembly pathway. These findings identify mesoscale trapping as an emergent kinetic regulatory mechanism in supramolecular polymerization.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e7258562"},"PeriodicalIF":16.9,"publicationDate":"2026-05-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147864899","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

Accelerated Proton Transfer Channel for Breaking the Bottlenecks of Activity and Stability at Industrial-Scale Anion Exchange Membrane Water Electrolysis. 加速质子转移通道突破工业规模阴离子交换膜电解活性和稳定性瓶颈。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2026-05-09 DOI: 10.1002/anie.1084711

Fuli Wang, Xintong Wei, Ning Yu, Mirabbos Hojamberdiev, Han Hu, Bin Dong, Shanshan Lu, Yongming Chai

{"title":"Accelerated Proton Transfer Channel for Breaking the Bottlenecks of Activity and Stability at Industrial-Scale Anion Exchange Membrane Water Electrolysis.","authors":"Fuli Wang, Xintong Wei, Ning Yu, Mirabbos Hojamberdiev, Han Hu, Bin Dong, Shanshan Lu, Yongming Chai","doi":"10.1002/anie.1084711","DOIUrl":"https://doi.org/10.1002/anie.1084711","url":null,"abstract":"Nickel-iron-based oxides are promising alkaline oxygen evolution reaction (OER) electrocatalysts, yet their practical implementation in anion exchange membrane (AEM) water electrolysis remains challenging for large-area membrane-electrode assembly (MEA) and stability due to complex synthesis and metal leaching issues. Herein, a scalable NiFeV0.5O electrocatalyst achieves the single-batch production of tens of grams and facilitates the fabrication of a 100 cm2 MEA using the catalyst-coated membrane (CCM) approach. Using various in situ characterization methods, we track the OER intermediates and identify the dynamic leaching and readsorption of VOx - species. We pioneer an operando rotating ring-disk electrode (RRDE) methodology with IrOx pH-sensing probes, which maps the interfacial acidity and demonstrates that these species elevate the local pH by 1.8 units via a hydrogen-bond-accelerated proton transfer channel. Experimental and computational analyses reveal that the readsorbed VOx - species are anchored via directional Fe─O─V bonds, suppressing Fe leaching by eight-fold compared to conventional NiFeO. Notably, when the gram-scale synthesized NiFeV0.5O is applied as an anode catalyst in a practical AEM water electrolyzer, it delivers 3.0 A cm-2 at a cell voltage of 1.88 V and exhibits remarkable stability at 1 A cm-2 over 500 h with a low decay rate of 0.12 mV h-1.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e1084711"},"PeriodicalIF":16.9,"publicationDate":"2026-05-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147864903","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

From Mechanism to Catalyst: Integrated Catalysts for Direct Electrosynthesis of Glycine Through an Oxime Pathway. 从机理到催化剂：肟途径直接电合成甘氨酸的集成催化剂。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2026-05-09 DOI: 10.1002/anie.9293384

Ying Zhou, Chaofan Wan, Qizhi Min, Xuan Wu, Ping Zhu, Yongfu Sun, Wenhua Zhang, Jinlong Yang

{"title":"From Mechanism to Catalyst: Integrated Catalysts for Direct Electrosynthesis of Glycine Through an Oxime Pathway.","authors":"Ying Zhou, Chaofan Wan, Qizhi Min, Xuan Wu, Ping Zhu, Yongfu Sun, Wenhua Zhang, Jinlong Yang","doi":"10.1002/anie.9293384","DOIUrl":"https://doi.org/10.1002/anie.9293384","url":null,"abstract":"The electrocatalytic synthesis of glycine from oxalic acid (H2C2O4) and hydroxylamine (NH2OH) involves a complex multi-step pathway comprising C-N coupling and multi-step selective protonation, making rational catalyst design a major challenge. In this work, by combining constant-potential density functional theory (DFT), the reaction mechanisms for the formation of glyoxylic oxime (GAO) from H2C2O4 and NH2OH on Pb surfaces, and its subsequent reduction to glycine on Cu surfaces are revealed. Guided by these mechanistic insights, we propose a set of criteria for designing integrated dual-site catalysts capable of catalyzing both GAO formation and selective protonation to glycine. Among the theoretically screened out integrated Pt1(Ir1, Ru1)/Pb(100) single atom catalysts, Pt1/Pb catalyst is synthesized experimentally, demonstrating high activity for glycine production. This study bridges fundamental mechanistic understanding with practical catalyst development for complex multi-step electrosynthesis.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e9293384"},"PeriodicalIF":16.9,"publicationDate":"2026-05-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147864886","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

Excited-State Pathway Switching via Reversible Structural Phase Transitions in Sb³⁺-Doped Cadmium Halides. Sb3+掺杂卤化镉的可逆结构相变激发态通路切换。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2026-05-09 DOI: 10.1002/anie.9627340

Zhe Tang, Binbin Fan, Chenxin Fan, Qingfeng Wei, Dandan Luo, Tingting Xue, Yan Su, Junsheng Chen

{"title":"Excited-State Pathway Switching via Reversible Structural Phase Transitions in Sb3+-Doped Cadmium Halides.","authors":"Zhe Tang, Binbin Fan, Chenxin Fan, Qingfeng Wei, Dandan Luo, Tingting Xue, Yan Su, Junsheng Chen","doi":"10.1002/anie.9627340","DOIUrl":"https://doi.org/10.1002/anie.9627340","url":null,"abstract":"Reversible control of structural phase transitions and luminescence remains a key challenge in organic-inorganic hybrid metal halides for stimuli-responsive photonic applications. Here, we report two new zero-dimensional (0D) Cd-based metal halides, (DFPD)6CdCl8 and (DFPD)2CdCl4·H2O (DFPD+ = 4,4-difluoropiperidine), in which Sb3+ doping enables distinct emission behaviors governed by coordination geometry. Combined spectroscopic studies and theoretical calculations reveal that Sb3+-doped (DFPD)6CdCl8 exhibits yellow emission with a large Stokes shift arising from triplet self-trapped exciton (3STE) emission, whereas Sb3+-doped (DFPD)2CdCl4·H2O displays excitation-dependent emission due to competing singlet STE (1STE) and 3STE states. This contrast originates from the different Cd-Cl coordination environments (octahedral vs. tetrahedral), which modulate the energy levels and transition dipole moments. Importantly, hydrochloric acid (HCl) and 4,4-difluoropiperidine induce fully reversible interconversion between the two structures, allowing dynamic switching between yellow and deep-orange emission. Based on this reversible luminescence, we further demonstrated applications in dynamic anti-counterfeiting and multilevel information encryption. This work establishes a coordination-structure-driven strategy for programmable emission in 0D hybrid metal halides.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e9627340"},"PeriodicalIF":16.9,"publicationDate":"2026-05-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147864905","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

Highly Selective On-Surface Synthesis of sp²/sp-Hybridized Heterochiral Triangular Nanorings. sp2/sp杂化杂手性三角形纳米环的高选择性表面合成。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2026-05-09 DOI: 10.1002/anie.6649441

Zhipeng Zhang, Xiaoyang Zhao, Tianchen Qin, Yue Huang, Liqian Liu, Jun Hu, Junfa Zhu, Tao Wang, Xinrui Miao

{"title":"Highly Selective On-Surface Synthesis of sp2/sp-Hybridized Heterochiral Triangular Nanorings.","authors":"Zhipeng Zhang, Xiaoyang Zhao, Tianchen Qin, Yue Huang, Liqian Liu, Jun Hu, Junfa Zhu, Tao Wang, Xinrui Miao","doi":"10.1002/anie.6649441","DOIUrl":"https://doi.org/10.1002/anie.6649441","url":null,"abstract":"A central challenge in on-surface synthesis of topologically unique carbon nanostructures lies in the precise and selective construction of triangular nanorings. Achieving the resulting chirality and the sp2/sp-hybridized state simultaneously from prochiral precursors is critical, yet immensely difficult. Here, we design an asymmetric α‑cyanostilbene derivative with aggregation‑induced emission properties as a prochiral building block to achieve deterministic pathway selection through controlling the substrate- and thermal-directed strategy, allowing for the targeted formation of heterochiral nanorings with defined sp2- and sp-hybridization on Ag(111). Direct thermal deposition onto a hot Ag(111) surface at 443 K drives a highly selective cyclotrimerization, yielding discrete sp2-hybridized heterochiral triangular nanorings. Subsequent annealing induces an elimination reaction, converting these rings into their sp-hybridized analogues while preserving chirality. In contrast, room-temperature deposition and postannealing predominantly produces linear chains. The structural evolution and selective reaction mechanisms are unequivocally characterized by scanning tunneling microscopy (STM), bond-resolution STM, synchrotron radiation photoemission spectroscopy (SRPES), and density functional theory (DFT) calculations. This work establishes a novel strategy for the precise synthesis of chiral triangular nanorings, revealing the critical role of surface-mediated conformational control and dynamic covalent bonding in determining product topology and chirality.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e6649441"},"PeriodicalIF":16.9,"publicationDate":"2026-05-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147864914","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

Unlocking Photocatalytic CO₂ Conversion to Ethylene Glycol by Microdroplet-Enabled Interfacial Electric Field. 利用微滴界面电场解锁光催化CO2转化为乙二醇。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2026-05-09 DOI: 10.1002/anie.6306355

Mengqiu Xu, Yutong Wang, Ran Tang, Zejiang Huang, Chen Wang, Cheng Liu, Licheng Wang, Liwu Zhang, Xuelu Wang, Qing Han, Gengfeng Zheng

{"title":"Unlocking Photocatalytic CO2 Conversion to Ethylene Glycol by Microdroplet-Enabled Interfacial Electric Field.","authors":"Mengqiu Xu, Yutong Wang, Ran Tang, Zejiang Huang, Chen Wang, Cheng Liu, Licheng Wang, Liwu Zhang, Xuelu Wang, Qing Han, Gengfeng Zheng","doi":"10.1002/anie.6306355","DOIUrl":"https://doi.org/10.1002/anie.6306355","url":null,"abstract":"The electrochemical carbon dioxide (CO2) reduction features attractive potentials of carbon neutrality and chemical upgrading, while the types of products from photocatalysis or electrocatalysis still remain limited. The conversion of CO2 into ethylene glycol, an important chemical that is typically produced by thermo-catalytic process, has not been achieved by photocatalysis or electrocatalysis. Herein, we demonstrate a microdroplet-enhanced photocatalytic strategy with a Pd-TiO2 catalyst, which allows for efficient conversion of CO2 into ethylene glycol with high selectivity. The electro-sprayed microdroplets provide a high interfacial electric field that facilitates deep reduction of CO2 into *CH3, as well as generation of reactive *OH intermediates to form CH3OH. The in situ formed CH3OH is further photo-catalytically activated to cleave a C-H bond to *CH2OH, followed by the C-C coupling to produce ethylene glycol. Under 1-sun illumination, the electro-sprayed microdroplets and Pd-TiO2 catalyst exhibited a high CO2-to-ethylene glycol conversion rate of 2985 µmol L-1 h-1, which significantly outperformed those by only photocatalysis or only electro-sprayed microdroplets, revealing the capability of combining multiple energy fields for tuning reaction pathways and advancing green synthesis.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e6306355"},"PeriodicalIF":16.9,"publicationDate":"2026-05-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147864879","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

Ultrafast Anion-Hopping Conduction in Organic Solvent via Imidazolium-Grafted Dynamic Ion-Conducting Spacers for Stable Non-Aqueous Flow Batteries. 稳定非水液流电池中咪唑接枝动态离子传导间隔剂在有机溶剂中的超快阴离子跳跃传导。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2026-05-09 DOI: 10.1002/anie.6160285

Pengzhu Gai, Hangyuan Wang, Qiang Chen, Hengqi Shi, Hongyan Cao, Yixing Wang, Ying Yu, Huidong Qian, Kang Huang, Zhi Xu

{"title":"Ultrafast Anion-Hopping Conduction in Organic Solvent via Imidazolium-Grafted Dynamic Ion-Conducting Spacers for Stable Non-Aqueous Flow Batteries.","authors":"Pengzhu Gai, Hangyuan Wang, Qiang Chen, Hengqi Shi, Hongyan Cao, Yixing Wang, Ying Yu, Huidong Qian, Kang Huang, Zhi Xu","doi":"10.1002/anie.6160285","DOIUrl":"https://doi.org/10.1002/anie.6160285","url":null,"abstract":"Non-aqueous flow batteries (NAFBs) require membranes with superior organic solvent resistance and high ionic conductivity in organic solvents to endure the corrosive effects inherent in non-aqueous electrolytes. Herein, we designed a highly organic-solvent-resistant imidazolium-grafted anion-exchange membrane (AEM) for NAFBs, realizing rapid anion hopping conduction in organic solvents. The membrane exhibited an ultrafast ionic conductivity as high as 2.1 mS cm-1 in DMF-based electrolyte which was much greater than that of the commercial Celgard membrane (only 0.45 mS·cm-1), coupled with exceptional barrier properties evidenced by ultralow active-species permeability values of 1.6 × 10-8 cm2 s-1 for 2,1,3-benzothiadiazole positive electrolyte and 3.8 × 10-9 cm2 s-1 for 10-methylphenothiazine negative electrolyte, respectively. Moreover, the membrane demonstrated outstanding stability in aggressive organic solvent, achieving an average energy efficiency (EE) over 66.1% for over 330 cycles at 5 mA cm-2 in a NAFB cell test, which far exceeded the commercial Celgard membrane (with only 70 cycles with an average EE of 48.8%). This research presents a strategic advance in next-generation membrane design for NAFBs with exceptional organic solvent resistance and high ionic conductivity.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e6160285"},"PeriodicalIF":16.9,"publicationDate":"2026-05-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147864891","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

Correction to "Electron Transfer Enhanced by a Minimal Energetic Driving Force at the Organic-Semiconductor Interface". 对“有机-半导体界面上最小能量驱动力增强的电子转移”的修正。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2026-05-09 DOI: 10.1002/anie.4364552

Hiroto Iwasaki, Keisuke Fujimoto, Koki Banno, Qing-Jun Shui, Yutaka Majima, Masaki Takahashi, Seiichiro Izawa

引用次数: 0

Alloy-Regulated Heterointerface Engineering for Kinetics-Driven Sulfur Redox in Li-S Batteries. Li-S电池动力学驱动硫氧化还原的合金调节异质界面工程。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2026-05-08 DOI: 10.1002/anie.6675271

Tongzhen Wang, Shuo Liu, Jie Yang, Yulei Li, Jiewu Cui, Yu Yao, Yan Yu, Yucheng Wu, Jiaqin Liu

{"title":"Alloy-Regulated Heterointerface Engineering for Kinetics-Driven Sulfur Redox in Li-S Batteries.","authors":"Tongzhen Wang, Shuo Liu, Jie Yang, Yulei Li, Jiewu Cui, Yu Yao, Yan Yu, Yucheng Wu, Jiaqin Liu","doi":"10.1002/anie.6675271","DOIUrl":"https://doi.org/10.1002/anie.6675271","url":null,"abstract":"Lithium-sulfur (Li-S) batteries offer exceptional theoretical energy density, yet their practical deployment is fundamentally constrained by sluggish sulfur redox kinetics and persistent shuttle of polysulfides. Here, we report a NiMo-alloy-assisted quantitative heterointerface engineering strategy that regulates the phase balance, interfacial abundance, and electronic coupling in Mo2C/MoC heterostructures. By tuning the Ni/Mo ratio as a continuous control parameter, NiMo incorporation drives controlled Mo2C→MoC phase reconstruction to maximize the density and accessibility of catalytically active Mo2C/MoC heterointerfaces, while the resulting NiMo domains primarily function as a structural modulator and metallic electron-transport pathway, complementing the conductive nitrogen-doped carbon framework. In situ/ex situ characterizations and density functional theory calculations reveal Mo2C/MoC heterointerfaces intrinsically exhibit the most favorable polysulfide adsorption strength and the lowest energy barriers for bidirectional sulfur conversion. As a result, Li-S cells equipped with the catalytic separator deliver a high reversible capacity of 1477.8 mAh g-1 at 0.1 C and sustain long-term cycling with an ultralow decay rate of 0.032% per cycle over 1000 cycles at 0.5 C, enabling an areal capacity of 15.2 mAh cm-2 at high sulfur loading. This work establishes a quantitative heterointerface design paradigm for regulating sulfur electrochemistry and provides general insights into heterostructure-enabled catalysis in metal-sulfur batteries.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e6675271"},"PeriodicalIF":16.9,"publicationDate":"2026-05-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147848954","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