Nature chemistry最新文献_第4页

Weaving two-dimensional peptide crystals 编织二维肽晶体。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-09-18 DOI: 10.1038/s41557-026-02252-0

Bidyut K. Kundu, Andy I. Nguyen

引用次数: 0

Forging ammonia with iron and light from water and nitrogen 用铁和光从水和氮中锻造氨。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-09-17 DOI: 10.1038/s41557-026-02253-z

Jens Uhlig

引用次数: 0

F-centre charge state and dynamism govern oxide electrocatalytic selectivity. f中心电荷态和动力学控制氧化物的电催化选择性。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-09-17 DOI: 10.1038/s41557-026-02256-w

Xiaoyuan Zhang, Danil Bukhvalov, Tiannan Su, Chenchen Fang, Liming Dai, Shuo San, Huiru Duan, Yaya Wang, Kai Liu, Junjie Cui, Yuxiang Hua, Liang Xue, Zhen Hou, Wenyao Zhang, Pan Xiong, Yongsheng Fu, Jingwen Sun, Junwu Zhu

{"title":"F-centre charge state and dynamism govern oxide electrocatalytic selectivity.","authors":"Xiaoyuan Zhang, Danil Bukhvalov, Tiannan Su, Chenchen Fang, Liming Dai, Shuo San, Huiru Duan, Yaya Wang, Kai Liu, Junjie Cui, Yuxiang Hua, Liang Xue, Zhen Hou, Wenyao Zhang, Pan Xiong, Yongsheng Fu, Jingwen Sun, Junwu Zhu","doi":"10.1038/s41557-026-02256-w","DOIUrl":"https://doi.org/10.1038/s41557-026-02256-w","url":null,"abstract":"Oxygen vacancies tune electronic structure and can steer electrocatalysis, yet their intrinsic charge state, identifiable as different F centres, remains a largely untapped lever. Here we devise a template-assisted, atmosphere-regulated route to ZrO2-x that keeps the crystal structure identical while varying the oxygen vacancy charge state, specifically electropositive F1 centres and electroneutral F2 centres, enabling a clean assessment of the impact on electrocatalytic selectivity. In situ electrochemical electron paramagnetic resonance tracking F-centre paramagnetism, together with in situ Raman of intermediate evolution, reveals that electroneutral F2 is not the primary adsorption site. Rather, its dynamic electronic compensation to adjacent sites is crucial to the adsorption and evolution of *OOH. This triggers the 2e- oxygen reduction reaction pathway. By contrast, electropositive F1 directly binds O2, causing O-O bond cleavage and subsequent quenching of the F1 centre. These findings establish charge-state-governed catalysis by distinct F centres and provide a new perspective for vacancy engineering in electrocatalyst design.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":" ","pages":""},"PeriodicalIF":24.5,"publicationDate":"2026-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148990558","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Nanoscale visualization of plasmon-enhanced hydrogen activation on a Pt(111) surface. Pt（111）表面等离子体增强氢活化的纳米级可视化。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-09-10 DOI: 10.1038/s41557-026-02245-z

Zhen-Feng Cai, Meghna A Manae, Zi-Xi Tang, Jun-Xian Zhang, Yao Zhang, Jeremy O Richardson, Naresh Kumar

{"title":"Nanoscale visualization of plasmon-enhanced hydrogen activation on a Pt(111) surface.","authors":"Zhen-Feng Cai, Meghna A Manae, Zi-Xi Tang, Jun-Xian Zhang, Yao Zhang, Jeremy O Richardson, Naresh Kumar","doi":"10.1038/s41557-026-02245-z","DOIUrl":"https://doi.org/10.1038/s41557-026-02245-z","url":null,"abstract":"Efficient H2 activation under mild conditions is crucial for achieving energy-efficient catalytic hydrogenation, but this remains a major challenge. Here we demonstrate nanoscale visualization of plasmon-enhanced H2 activation on Pt(111) at room temperature under visible light by employing a combination of spectroscopic and modelling methods. In situ tip-enhanced Raman spectroscopy tracked H2 activation through H-assisted desorption of an oligomeric phenylene-ethynylene thiolate reporter, while hyperspectral imaging revealed ~20% enhancement in the 180-300 nm region around the near field. Spectroscopic evidence and finite element method simulations excluded the plasmonic heating effect, whereas quantum calculations showed that hot electrons generated in the tip-enhanced Raman spectroscopy near field can efficiently drive H2 dissociation via an indirect transfer mechanism. Notably, we found that activated H atoms propagate hundreds of nanometres beyond the near field through a collective crowd effect. These findings provide mechanistic insights into plasmon-enhanced H2 activation on Pt surfaces and suggest future opportunities for energy-efficient catalytic hydrogenation.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":" ","pages":""},"PeriodicalIF":24.5,"publicationDate":"2026-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148930430","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Ionic clusters as high-connectivity secondary building units for crystalline porous organic salts. 离子团簇作为结晶多孔有机盐的高连通性二级构建单元。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-09-08 DOI: 10.1038/s41557-026-02248-w

Yu-Lin Lu, Yishuo Chen, Hang Qu, Laiyu Zhang, Megan O'Shaughnessy, Thomas Fellowes, Andrew I Cooper

{"title":"Ionic clusters as high-connectivity secondary building units for crystalline porous organic salts.","authors":"Yu-Lin Lu, Yishuo Chen, Hang Qu, Laiyu Zhang, Megan O'Shaughnessy, Thomas Fellowes, Andrew I Cooper","doi":"10.1038/s41557-026-02248-w","DOIUrl":"https://doi.org/10.1038/s41557-026-02248-w","url":null,"abstract":"The solid-state assembly of crystalline porous materials is dictated by a balance between primary node-linker interactions and other weaker intermolecular forces. Metal-organic frameworks (MOFs) exploit highly directional and rigid coordination bonds that outweigh competing packing effects. This allows high-connectivity secondary building units (SBUs) to be assembled into a diverse range of architectures. By contrast, molecular crystals comprise weaker intermolecular interactions, making it challenging to realize porous packings with the highly connected reticular topologies achieved in MOFs. Here we introduce Coulombic aggregation as a means to generate primary SBU motifs. By suppressing intermolecular dispersion interactions, ammonium halide ion pairs aggregate into discrete multinuclear clusters that function as non-metal SBUs. Coupled with multitopic three-dimensional linkers, these ionic clusters create extended non-metal organic frameworks with diverse topologies, large voids and polar channels. This study extends reticular chemistry from directional chemical bonds to 'soft' ionic interactions, opening pathways to new porous materials and principles of solid-state assembly.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":" ","pages":""},"PeriodicalIF":24.5,"publicationDate":"2026-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148912984","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Directed heterogeneous hydride transfer enables selective CO2 reduction using a Janus palladium membrane electrode 定向异质氢化物转移使选择性二氧化碳减少使用Janus钯膜电极

IF 21.8 1区化学

Nature chemistry Pub Date : 2026-09-07 DOI: 10.1038/s41557-026-02243-1

Xiaosong Hu (胡小松), William Boyd, Feihu Wang (王飞虎), Aaron Diefendorf, Owen Cowling, Yujie Sun (孙宇杰)

{"title":"Directed heterogeneous hydride transfer enables selective CO2 reduction using a Janus palladium membrane electrode","authors":"Xiaosong Hu \u0000 (胡小松), William Boyd, Feihu Wang \u0000 (王飞虎), Aaron Diefendorf, Owen Cowling, Yujie Sun \u0000 (孙宇杰)","doi":"10.1038/s41557-026-02243-1","DOIUrl":"https://doi.org/10.1038/s41557-026-02243-1","url":null,"abstract":"Electrochemical CO2 reduction is typically constrained by proton-coupled electron transfer, which intrinsically intertwines CO2 conversion with the competing H2 evolution reaction. Here we introduce a Janus palladium membrane electrode that circumvents proton-coupled electron transfer by enabling selective CO2 reduction through heterogeneous hydride transfer. The membrane spatially separates hydrogen generation from CO2 reduction and independently polarizes the CO2-facing interface, converting permeated hydrogen atoms into Pd–H species with tunable hydricity. This design sustains directional hydride flux from water to CO2, enabling highly selective formate production under mild cathodic polarization. We achieve excellent Faradaic efficiencies and turnover frequencies in aqueous electrolytes, while isotope labelling experiments confirm hydride transfer as the dominant reaction pathway. Continuous hydrogen delivery stabilizes a hydrogen-rich surface of the electrode, suppressing CO formation and enabling stable operation. This electrode’s success for CO2 reduction in both aqueous and fully aprotic electrolytes offers a general route to access heterogeneous hydride reactivity beyond proton-mediated electrocatalysis.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"78 1","pages":""},"PeriodicalIF":21.8,"publicationDate":"2026-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148899599","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Lower-temperature bulk depolymerization of commercial polymethacrylates. 商品聚甲基丙烯酸酯的低温本体解聚。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-09-02 DOI: 10.1038/s41557-026-02232-4

Richard Whitfield, Victoria Lohmann, Mikhail Agrachev, Hongsik Kim, Hyun Suk Wang, Nethmi De Alwis Watuthanthrige, Nghia P Truong, Tae-Lim Choi, Gunnar Jeschke, Athina Anastasaki

{"title":"Lower-temperature bulk depolymerization of commercial polymethacrylates.","authors":"Richard Whitfield, Victoria Lohmann, Mikhail Agrachev, Hongsik Kim, Hyun Suk Wang, Nethmi De Alwis Watuthanthrige, Nghia P Truong, Tae-Lim Choi, Gunnar Jeschke, Athina Anastasaki","doi":"10.1038/s41557-026-02232-4","DOIUrl":"https://doi.org/10.1038/s41557-026-02232-4","url":null,"abstract":"Chemical recycling back to monomer represents an attractive methodology to tackle plastic waste. However, current reports focus on either thermally unstable 'designer' polymers or highly diluted solution depolymerizations. Here we report a simple, yet efficient, bulk main-chain scission pathway, whereby the presence of N-hydroxyphthalimides triggers a hydrogen-atom-transfer reaction on the polymer backbone, followed by the rapid and near-quantitative depolymerization of polymethacrylates. Notably, this strategy can be directly applied to crude commercial polymers, does not rely on preinstalled end-groups or sacrificial co-monomers, operates at relatively low temperatures in the absence of light irradiation and precludes the use of a solvent, therefore enabling direct isolation of pristine monomers in high yields (∼90%). The methodology is compatible with polymethacrylates synthesized by either anionic, free radical or controlled radical polymerization and can also be applied to ultrahigh-molecular-weight materials (>106 Da).","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":" ","pages":""},"PeriodicalIF":24.5,"publicationDate":"2026-09-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148881294","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Palladium-triggered bioorthogonal phenylalanine decaging. 钯引发的生物正交苯丙氨酸降解。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-09-02 DOI: 10.1038/s41557-026-02226-2

Yuchao Zhu, Shibo Liu, Shan Qin, Xin Wang, Yuan Liu, Xianrui Zhang, Ye Shan, Xinyuan Fan, Peng R Chen

{"title":"Palladium-triggered bioorthogonal phenylalanine decaging.","authors":"Yuchao Zhu, Shibo Liu, Shan Qin, Xin Wang, Yuan Liu, Xianrui Zhang, Ye Shan, Xinyuan Fan, Peng R Chen","doi":"10.1038/s41557-026-02226-2","DOIUrl":"10.1038/s41557-026-02226-2","url":null,"abstract":"Phenylalanine (Phe) orchestrates protein interfacial hydrophobicity and π-driven interactions that are critical for diverse biological processes. Its nonpolar architecture, however, precludes traditional heteroatom-dependent reactions, leaving its functional manipulation in living systems unresolved. Here, by systematically evaluating exogenous heteroatom-based (X = O, N, B or I) caging groups under physiological conditions, we present a haloatom-assisted decaging strategy that uses iodine to cage Phe's side chain. This blockade can be tracelessly rescued through palladium-triggered bioorthogonal decaging. Through precise modulation, the haloatom-assisted decaging strategy enables: unmasking fluorophore activity, directing peptide disassembly, reactivating protein-protein interactions and rewiring cell-cell recognition. Using genetic code expansion, we site-specifically incorporated iodinated Phe into HER2-targeting affibodies for dynamic control of ligand-receptor interaction on the cell surface. Moreover, Phe decaging permits temporally controlled reshaping of antigenic peptide immunogenicity on tumour cells, thereby rewiring tumour-T cell engagement. We further optimized the decaging chemistry in cell lysates as well as inside living cells, which unlocks the possibility of chemically manipulating ubiquitous and functionally critical nonpolar groups in living systems.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":" ","pages":""},"PeriodicalIF":24.5,"publicationDate":"2026-09-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148881357","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Programmable alkene skeleton construction via switchable radical and organometallic sorting. 可编程烯烃骨架结构通过可切换的自由基和有机金属分类。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-09-01 DOI: 10.1038/s41557-026-02242-2

Chengmi Huang, Shuang Deng, Dong Wu, Shiyang Wang, Yangyang Li, Xiaotian Qi, Guoyin Yin

{"title":"Programmable alkene skeleton construction via switchable radical and organometallic sorting.","authors":"Chengmi Huang, Shuang Deng, Dong Wu, Shiyang Wang, Yangyang Li, Xiaotian Qi, Guoyin Yin","doi":"10.1038/s41557-026-02242-2","DOIUrl":"https://doi.org/10.1038/s41557-026-02242-2","url":null,"abstract":"The programmable synthesis of complex alkene skeletons, including regioisomers, stereoisomers and conjugated homologues in a single operation, is a long-standing goal in synthetic chemistry, given the profound influence of these structural features on molecular function. Traditional methods typically rely on predesigned substrates or rigid reaction pathways, which often restrict structural diversity. Here we report a nickel-catalysed sequential coupling of alkynes, organohalides and a diboron reagent. This method not only simultaneously achieves regioselective and unique stereoselective modulation in alkyne difunctionalization, affording uncommon 1,2-trans and 2,1-cis alkenes, but also accomplishes the construction of conjugated homologues via the controlled incorporation of two alkynes, thereby achieving the rare divergent synthesis of two conjugated diene products. Mechanistic studies reveal that the electronic properties of the ligands regulate the generation of organometallic species versus radicals, while the intrinsic metal-binding ability of the various radicals further modulates their reactivity, collectively governing product selectivity.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":" ","pages":""},"PeriodicalIF":24.5,"publicationDate":"2026-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148875033","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Thalidomide and targeted protein degradation 沙利度胺和靶向蛋白降解

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-08-28 DOI: 10.1038/s41557-026-02234-2

Connor Delaney

引用次数: 0