Nature Catalysis最新文献_第2页

Iron-based single-atom catalysts for selective ammoxidation of C(sp3)–H bonds and oxidative C–C cleavage reactions 选择性氨氧化C(sp3) -H键和氧化C - C裂解反应的铁基单原子催化剂

IF 44.6 1区化学

Nature Catalysis Pub Date : 2026-04-08 DOI: 10.1038/s41929-026-01513-y

Zhuang Ma (, ), Nils Rockstroh, Zupeng Chen (, ), Vishakha Goyal, Chakreshwara Kuloor, Stephan Bartling, Zdeněk Baďura, Jabor Rabeah, Lin Dong (, ), Henrik Lund, Bing Nan (, ), Radek Zbořil, Rajenahally V. Jagadeesh, Matthias Beller

{"title":"Iron-based single-atom catalysts for selective ammoxidation of C(sp3)–H bonds and oxidative C–C cleavage reactions","authors":"Zhuang Ma \u0000 (, ), Nils Rockstroh, Zupeng Chen \u0000 (, ), Vishakha Goyal, Chakreshwara Kuloor, Stephan Bartling, Zdeněk Baďura, Jabor Rabeah, Lin Dong \u0000 (, ), Henrik Lund, Bing Nan \u0000 (, ), Radek Zbořil, Rajenahally V. Jagadeesh, Matthias Beller","doi":"10.1038/s41929-026-01513-y","DOIUrl":"10.1038/s41929-026-01513-y","url":null,"abstract":"Ammoxidation of methylarenes using ammonia and air is the main method for the synthesis of aromatic nitriles in the chemical industry. Despite significant efforts in industry and academia, no general and selective catalyst based on less toxic and earth-abundant metals has been developed for this reaction. Here we report a single-atom iron-based material (Fe@BNC-800-L1) with Fe–N5–Bx configuration as an efficient sp3-hybridized C–H- and C–C bond oxidation catalyst. Due to the presence of Fe3+, B and N species, which are co-embedded in the micro-mesoporous carbon matrix, these materials show excellent activity for ammoxidation of methyl-substituted (hetero)arenes. Furthermore, highly selective C–C bond cleavage reactions of alkylarenes are presented, which complement the toolbox for nitrile synthesis. The generality of this presented Fe-based ammoxidation methodology is showcased by the straightforward and selective synthesis of >60 functionalized and structurally diverse nitriles, which are important precursors and key intermediates in organic synthesis with many applications in life sciences and industry. Catalytic ammoxidation of methylarenes to nitriles is industrially relevant, yet current systems rely on noble metals or harsh conditions. Now an Fe-based single-atom catalyst in B,N-doped carbon enables selective C(sp³)–H ammoxidation and C–C cleavage using molecular oxygen and ammonia.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"9 4","pages":"389-403"},"PeriodicalIF":44.6,"publicationDate":"2026-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.comhttps://www.nature.com/articles/s41929-026-01513-y.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147631173","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Favourable hydrogenation of pyridines via H2-adsorption modulation on Ni nanoparticles in dealuminated Beta zeolite 脱铝β沸石中Ni纳米颗粒h2吸附调制对吡啶的有利加氢作用

IF 44.6 1区化学

Nature Catalysis Pub Date : 2026-04-06 DOI: 10.1038/s41929-026-01521-y

Huixin Wu, Qian Xiang, Liang Wang, Hai Wang, Qingsong Luo, Yating Lv, Lifan Deng, Yuexin Wu, Yu Hui, Rui Tang, Wentao Yuan, Yong Wang, Qing Wu, Xiao-Ming Cao, Liang Wang, Feng-Shou Xiao

{"title":"Favourable hydrogenation of pyridines via H2-adsorption modulation on Ni nanoparticles in dealuminated Beta zeolite","authors":"Huixin Wu, Qian Xiang, Liang Wang, Hai Wang, Qingsong Luo, Yating Lv, Lifan Deng, Yuexin Wu, Yu Hui, Rui Tang, Wentao Yuan, Yong Wang, Qing Wu, Xiao-Ming Cao, Liang Wang, Feng-Shou Xiao","doi":"10.1038/s41929-026-01521-y","DOIUrl":"10.1038/s41929-026-01521-y","url":null,"abstract":"Hydrogenation of pyridines is particularly challenging because their strong coordination to metal sites hinders hydrogen adsorption and can poison the catalysts. Here we show that Ni nanoparticles (NPs) within zeolite crystals can overcome this problem, owing to a network of micropores that features a greater proportion of free Ni sites for hydrogen adsorption even in the presence of pyridines. As a result, a high activity was achieved under mild conditions, substantially outperforming those of the commercial Raney Ni and conventional supported Ni catalysts. In addition, Ni leaching from the Ni NPs within the zeolite crystals was effectively hindered under the reaction conditions, achieving excellent stability. The versatility of the approach was shown by synthesizing Pd NP analogues, which showed improved activity compared with the conventional supported Pd catalysts. Pyridine hydrogenation on supported metal particles is a powerful yet challenging synthetic transformation due to the strong coordinating effect of pyridine that limits hydrogen adsorption and activation. Here the authors adopt dealuminated Beta zeolite to entrap nickel nanoparticles and use the porosity of the support to effectively modulate pyridine and hydrogen activation.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"9 4","pages":"424-433"},"PeriodicalIF":44.6,"publicationDate":"2026-04-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147620368","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

Systematically exploring yeast metabolism through retrobiosynthesis and deep learning 通过逆转录生物合成和深度学习系统地探索酵母代谢

IF 44.6 1区化学

Nature Catalysis Pub Date : 2026-04-06 DOI: 10.1038/s41929-026-01523-w

Ke Wu, Haohao Liu, Yao Zhou, Manda Sun, Runze Mao, Yindi Jiang, Eduard J. Kerkhoven, Yu Chen, Jens Nielsen, Hongting Tang, Feiran Li

{"title":"Systematically exploring yeast metabolism through retrobiosynthesis and deep learning","authors":"Ke Wu, Haohao Liu, Yao Zhou, Manda Sun, Runze Mao, Yindi Jiang, Eduard J. Kerkhoven, Yu Chen, Jens Nielsen, Hongting Tang, Feiran Li","doi":"10.1038/s41929-026-01523-w","DOIUrl":"10.1038/s41929-026-01523-w","url":null,"abstract":"A systematic understanding of cellular metabolism is essential for engineering yeast and uncovering the principles of metabolic robustness and evolution, yet much of its metabolic space remains unexplored. Although yeast genome-scale metabolic models have been reconstructed and curated for over two decades, more than 90% of the yeast metabolome remains uncovered. Here, to address this gap, we have developed an integrated workflow that combines retrobiosynthesis, deep learning-based enzyme annotation and enzyme–substrate prediction to systematically explore yeast underground metabolism. Using the framework, we reconstruct a yeast metabolic twin model, Yeast-MetaTwin, comprising 16,244 metabolites, 1,976 metabolic genes and 59,865 reactions. The model reveals systematic differences in Km distributions between the known and underground networks and identifies key hub metabolites linking the underground network. Moreover, Yeast-MetaTwin predicts by-product formation in yeast cell factories, and we experimentally validate two genes converting geraniol to geranial during geraniol biosynthesis. Cellular underground metabolism plays crucial roles in enzyme promiscuity, metabolism and biological evolution, but it has hardly been investigated. Here the authors combine retrobiosynthesis with deep learning enzyme annotation and enzyme–substrate prediction methods to explore it, reconstructing the yeast metabolic twin model, Yeast-MetaTwin.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"9 4","pages":"434-447"},"PeriodicalIF":44.6,"publicationDate":"2026-04-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147620370","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

A high-flux membrane electrode assembly for CO2 electroreduction to 4.5 M formate with over 8,000 h stability 一种高通量膜电极组件，用于CO2电还原到4.5 M甲酸盐，稳定性超过8,000 h

IF 37.8 1区化学

Nature Catalysis Pub Date : 2026-04-03 DOI: 10.1038/s41929-026-01524-9

Jing-Jing Li, Hong-Juan Wang, Chao Zhang, Yu Li, Jiqing Jiao, Lin-Lin Wang, Cuo Wu, Di-Chang Zhong, Zhen-Yu Wu, Zi-You Yu, Tong-Bu Lu

引用次数: 0

Enantioselective C(sp3)–C(sp3) bond formation by synergistic thiamine-dependent radical biocatalysis and photoredox catalysis 协同硫胺素依赖的自由基生物催化和光氧化还原催化形成对映选择性C(sp3) -C （sp3）键

IF 44.6 1区化学

Nature Catalysis Pub Date : 2026-04-02 DOI: 10.1038/s41929-026-01515-w

Jianlin Chun, Yuyan Bao, Qiaoyu Zhang, Xueli Hou, Zhouping Wu, Hailong Sun, Zhongqiu Xing, Bin Chen, Zihan Zhang, Yue Zhao, Jiahai Zhou, Binju Wang, Xiaoqiang Huang

{"title":"Enantioselective C(sp3)–C(sp3) bond formation by synergistic thiamine-dependent radical biocatalysis and photoredox catalysis","authors":"Jianlin Chun, Yuyan Bao, Qiaoyu Zhang, Xueli Hou, Zhouping Wu, Hailong Sun, Zhongqiu Xing, Bin Chen, Zihan Zhang, Yue Zhao, Jiahai Zhou, Binju Wang, Xiaoqiang Huang","doi":"10.1038/s41929-026-01515-w","DOIUrl":"10.1038/s41929-026-01515-w","url":null,"abstract":"Radical C(sp3)–C(sp3) bond formation has emerged as a promising strategy for constructing molecules rich in C(sp3)–stereocentres. However, achieving chemo- and enantioselective recombination of two prochiral alkyl radicals remains a substantial challenge. Here we synergistically repurpose a thiamine-dependent benzoylformate decarboxylase (PpBFD) with a photoinduced radical process, unlocking unnatural photobiocatalytic C(sp3)–C(sp3) bond formation. This system converts simple cinnamyl aldehydes into enantioenriched carboxylic acids bearing valuable β-, or β,γ-C(sp3)–stereocentres, a new-to-nature transformation that is difficult to achieve with conventional methods. Through directed evolution, we precisely control alkyl radicals to achieve stereoselective C(sp3)–C(sp3) bond formation (38 examples, up to 96% e.e. and up to 91:9 d.r.). This work demonstrates that the reshaping of a different class of thiamine-dependent enzymes can expand the repertoire of radical biocatalysis. Radical C(sp3)–C(sp3) bond formation with stereocontrol is challenging. Now, photoredox catalysis and repurposed thiamine-dependent enzymes are combined to couple cinnamyl aldehydes with benzylic radicals, yielding enantioenriched carboxylic acids bearing one or even two stereocentres.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"9 4","pages":"414-423"},"PeriodicalIF":44.6,"publicationDate":"2026-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147611864","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

Dynamics of a Cu/ZnO/Al2O3 catalyst revealed by operando transmission electron microscopy during CO2 hydrogenation Cu/ZnO/Al2O3催化剂在CO2加氢过程中的动力学

IF 44.6 1区化学

Nature Catalysis Pub Date : 2026-04-01 DOI: 10.1038/s41929-026-01514-x

Maxime Boniface, Thomas Götsch, Jinhu Dong, Jutta Kröhnert, Elias Frei, Annette Trunschke, Robert Schlögl, Beatriz Roldan Cuenya, Thomas Lunkenbein

{"title":"Dynamics of a Cu/ZnO/Al2O3 catalyst revealed by operando transmission electron microscopy during CO2 hydrogenation","authors":"Maxime Boniface, Thomas Götsch, Jinhu Dong, Jutta Kröhnert, Elias Frei, Annette Trunschke, Robert Schlögl, Beatriz Roldan Cuenya, Thomas Lunkenbein","doi":"10.1038/s41929-026-01514-x","DOIUrl":"10.1038/s41929-026-01514-x","url":null,"abstract":"Cu/ZnO/Al2O3 catalysts are the industrial standard for methanol synthesis. Their high activity stems from the synergy between Cu and Zn, but their precise structure under CO2 hydrogenation conditions remains unknown. Here we show, using operando transmission electron microscopy, that the formation of ZnOx overlayers and CuZn surface alloys on Cu surfaces can be reversible and is mediated by the operating temperature and the chemical potential of the gas phase. Lower temperatures and more oxidative conditions lead to thicker ZnOx overlayers. At elevated temperatures, the overlayer coverage opens, exposing Cu nanoparticle surfaces to the feed and enabling CO2 activation. Furthermore, we show that CuZn alloys are transient species and are re-oxidized by H2O formed during the reaction. This implies that, in CO2 hydrogenation conditions, CuZn and Cu–ZnO surface states may coexist and continuously convert into one another as the local chemical potential oscillates throughout steady-state operation. Maintaining this fluctuation might be critical to the lifetime and performance of the catalyst. Cu/ZnO/Al2O3 catalysts are used in industry for methanol synthesis and the water–gas shift reaction, but some of their structural features under operation remain elusive. Now operando transmission electron microscopy reveals the dynamic nature of ZnOx overlayers upon temperature cycling and proposes a reaction mechanism that is build on the reversible interconversion of Cu–ZnO surface and CuZn surface alloys on copper, which is considered to be mediated by the reaction conditions.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"9 4","pages":"404-413"},"PeriodicalIF":44.6,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.comhttps://www.nature.com/articles/s41929-026-01514-x.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147586017","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Catalysis shines on arsenic minerals 催化作用在砷矿物上发光

IF 44.6 1区化学

Nature Catalysis Pub Date : 2026-03-27 DOI: 10.1038/s41929-026-01516-9

Jan-Stefan Völler

引用次数: 0

Diastereocontrolling macrocylization Diastereocontrolling macrocylization

IF 44.6 1区化学

Nature Catalysis Pub Date : 2026-03-27 DOI: 10.1038/s41929-026-01517-8

Francesco Zamberlan

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Reality check on propane dehydrogenation 丙烷脱氢的现实检查

IF 44.6 1区化学

Nature Catalysis Pub Date : 2026-03-27 DOI: 10.1038/s41929-026-01510-1

Giovanni Pampararo, Michiel Dusselier

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Enabling open and FAIR catalysis data with standardized data structures 使用标准化的数据结构启用开放和公平的催化数据

IF 44.6 1区化学

Nature Catalysis Pub Date : 2026-03-27 DOI: 10.1038/s41929-026-01508-9

Julia Schumann, Hampus Näsström, Michael Götte, Lauri Himanen, Abdulrhman Moshantaf, Markus Scheidgen, José A. Márquez, Claudia Draxl, Annette Trunschke

引用次数: 0