Nature Catalysis最新文献_第8页

A polyheteroatomic Diels–Alderase 多杂原子双醛酶

IF 44.6 1区化学

Nature Catalysis Pub Date : 2025-05-28 DOI: 10.1038/s41929-025-01351-4

Jan-Stefan Völler

引用次数: 0

Chiral cyclopropanes with light in confined space 手性环丙烷与密闭空间中的光

IF 44.6 1区化学

Nature Catalysis Pub Date : 2025-05-28 DOI: 10.1038/s41929-025-01345-2

Magdalena Walewska-Królikiewicz, Dorota Gryko

引用次数: 0

Modulation to probe the interface 调制探测接口

IF 44.6 1区化学

Nature Catalysis Pub Date : 2025-05-28 DOI: 10.1038/s41929-025-01356-z

Marçal Capdevila-Cortada

引用次数: 0

Unlocking iron spin states for oxygen reduction 解锁铁的自旋态来还原氧

IF 44.6 1区化学

Nature Catalysis Pub Date : 2025-05-28 DOI: 10.1038/s41929-025-01343-4

Jaehyuk Shim, Yung-Eun Sung

引用次数: 0

Ordered single active sites for cascade hydrogenation and hydroformylation reactions 级联加氢和氢甲酰化反应的有序单活性位点

IF 44.6 1区化学

Nature Catalysis Pub Date : 2025-05-26 DOI: 10.1038/s41929-025-01346-1

Xiaojun Lu, Jiazhen Wu, Xinyi He, Zichuang Li, Yangfan Lu, Wenqian Li, Jiang Li, Miao Xu, Yanpeng Qi, Qing Zhang, Yijia Liu, Meng Du, Toshio Kamiya, Hideo Hosono, Fusheng Pan, Jie-Sheng Chen, Tian-Nan Ye

{"title":"Ordered single active sites for cascade hydrogenation and hydroformylation reactions","authors":"Xiaojun Lu, Jiazhen Wu, Xinyi He, Zichuang Li, Yangfan Lu, Wenqian Li, Jiang Li, Miao Xu, Yanpeng Qi, Qing Zhang, Yijia Liu, Meng Du, Toshio Kamiya, Hideo Hosono, Fusheng Pan, Jie-Sheng Chen, Tian-Nan Ye","doi":"10.1038/s41929-025-01346-1","DOIUrl":"10.1038/s41929-025-01346-1","url":null,"abstract":"Metal single-atom catalysts offer improved activity and selectivity due to their unique electronic and coordination properties compared with bulk metals. However, many single-atom catalysts suffer from randomly dispersed active sites and limited electron-donating ability due to bonding with electronegative elements or less reactive metals. Here we demonstrate that Mg-rich intermetallic Mg29TM4 (TM = Pd, Rh, Ir, Pt) nanocatalysts overcome these limitations. These materials feature periodically dispersed, electron-rich single-atom sites of noble metals within a uniform chemical environment. Mg29TM4 exhibits high activity and selectivity in C2H2 semihydrogenation (Mg29Pd4) and olefin hydroformylation (Mg29Rh4), with Mg29Rh4 achieving high regioselectivity for branched aldehydes (branched:linear > 200:1). Kinetic and density functional theory studies suggest that the Mg–TM ensemble enables precise control over carbon–carbon multiple bond adsorption and activation, enhancing both activity and selectivity. Furthermore, the ternary Mg29Pd1.3Rh2.7 catalyst, with its synergistic Mg–Pd and Mg–Rh dual single-atom sites, efficiently catalyses a cascade reaction involving phenylacetylene hydrogenation followed by hydroformylation. Single-atom catalysts commonly present a random distribution of the active metal centres. Now a series of Mg-rich intermetallic compounds is introduced to enable ordered dispersed active metals. Furthermore, a cascade process is demonstrated on Mg29Pd1.3Rh2.7, where Pd sites catalyse the semihydrogenation of phenylacetylene with subsequent hydroformylation on Rh sites.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 6","pages":"536-547"},"PeriodicalIF":44.6,"publicationDate":"2025-05-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144137205","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

SnSe nanosheets with Sn vacancies catalyse H2O2 production from water and oxygen at ambient conditions 具有Sn空位的SnSe纳米片在环境条件下催化水和氧生成H2O2

IF 44.6 1区化学

Nature Catalysis Pub Date : 2025-05-23 DOI: 10.1038/s41929-025-01335-4

Xinyue Zhang, Yangyang Wan, Yi Wen, Yingcai Zhu, Hong Liu, Jiaxiang Qiu, Zhanpeng Zhu, Zhongti Sun, Xiang Gao, Shulin Bai, Yuqiao Zhang, Long Zhang, Xiaohong Yan, Jianming Zhang, Yong Liu, Shun Li, Li-Dong Zhao

{"title":"SnSe nanosheets with Sn vacancies catalyse H2O2 production from water and oxygen at ambient conditions","authors":"Xinyue Zhang, Yangyang Wan, Yi Wen, Yingcai Zhu, Hong Liu, Jiaxiang Qiu, Zhanpeng Zhu, Zhongti Sun, Xiang Gao, Shulin Bai, Yuqiao Zhang, Long Zhang, Xiaohong Yan, Jianming Zhang, Yong Liu, Shun Li, Li-Dong Zhao","doi":"10.1038/s41929-025-01335-4","DOIUrl":"10.1038/s41929-025-01335-4","url":null,"abstract":"Hydrogen peroxide (H2O2) is a vital industrial chemical and sustainable energy carrier. However, achieving a simple, efficient and cost-effective synthesis under mild conditions remains an important challenge. Here we show that SnSe nanosheets with Sn vacancies can directly catalyse H2O2 production from H2O and O2 under ambient conditions, without additional energy inputs (for example, light and electricity), cocatalysts or sacrificial reagents. This approach achieves an optimal H2O2 production rate of ~2.6 mmol g−1 h−1 at 40 °C and maintains long-term stable production (~0.3 mmol l−1) in a continuous-flow reactor for over 50 h at room temperature. Experimental and theoretical analyses reveal that this unique thermocatalytic effect arises from a dynamic process involving Sn vacancy defect-induced sequential dissociation of H2O and activation of O2 molecules, along with reversible surface restructuring of the SnSe nanosheets to release H2O2. Our findings offer a notably simple, highly efficient and entirely green strategy for H2O2 production, with broader implications in other catalytic reactions involving water activation. H2O2 is a commodity chemical produced in industry via the anthraquinone process from H2 and O2. Now a heterogeneous catalysis approach is presented in which H2O2 is synthesized from H2O and O2 on defective SnSe nanosheets at ambient conditions.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 5","pages":"465-475"},"PeriodicalIF":44.6,"publicationDate":"2025-05-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144122592","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

Selective formaldehyde condensation on phosphorus-rich copper catalyst to produce liquid C3+ chemicals in electrocatalytic CO2 reduction 选择性甲醛在富磷铜催化剂上缩合生成液态C3+化学物电催化CO2还原

IF 44.6 1区化学

Nature Catalysis Pub Date : 2025-05-22 DOI: 10.1038/s41929-025-01341-6

Minjun Choi, Sooan Bae, Yeongin Kim, Youjin Lee, Mokyeon Cho, Sinwoo Kang, Jaeyoung Lee

{"title":"Selective formaldehyde condensation on phosphorus-rich copper catalyst to produce liquid C3+ chemicals in electrocatalytic CO2 reduction","authors":"Minjun Choi, Sooan Bae, Yeongin Kim, Youjin Lee, Mokyeon Cho, Sinwoo Kang, Jaeyoung Lee","doi":"10.1038/s41929-025-01341-6","DOIUrl":"10.1038/s41929-025-01341-6","url":null,"abstract":"Recent advancements in the CO2 reduction reaction (CO2RR) target multicarbon chemical production and scalable electrode designs for industrial applications. Here we introduce a zero-gap cell utilizing humidified gas-phase CO2 and circulated alkaline media, achieving a Faradaic efficiency of 66.9% for C3+ products and a current density of −1,100 mA cm−2. In situ spectroscopic analyses revealed formaldehyde as a key intermediate formed on copper oxide/hydroxide interfaces derived from a phosphorus-rich copper catalyst. Unlike conventional pathways based on dimerization of CO intermediates, our study selectively produces liquid-phase multicarbon products because of autonomous local pH variations under a weak alkaline microenvironment, with allyl alcohol as the dominant C3+ product. The high selectivity and efficiency for liquid products provide a substantial advantage for storage and transport, highlighting the scalability and practical feasibility of our approach, which offers a potential economically viable solution for CO2 utilization. This development encourages the adoption of CO2RR technologies in iron–steel and petrochemical industries to mitigate greenhouse gas emissions. Electrocatalytic CO2 reduction has largely been limited to C1 and C2 products, especially at high current densities. Here, a Faradaic efficiency of 67% is reported for C3+ products from CO2 at 1.1 A cm−2 via a formaldehyde condensation mechanism on a phosphorus-rich copper catalyst.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 5","pages":"476-486"},"PeriodicalIF":44.6,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.comhttps://www.nature.com/articles/s41929-025-01341-6.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144113527","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

Cobalt-catalysed alkene hydronitration enabled by anomeric nitroamide 异头氮酰胺使钴催化烯烃加氢化

IF 44.6 1区化学

Nature Catalysis Pub Date : 2025-05-21 DOI: 10.1038/s41929-025-01336-3

Yu Wang, Marcell M. Bogner, Jake B. Bailey, Lauren N. Grant, Milan Gembicky, Paul F. Richardson, Phil S. Baran

{"title":"Cobalt-catalysed alkene hydronitration enabled by anomeric nitroamide","authors":"Yu Wang, Marcell M. Bogner, Jake B. Bailey, Lauren N. Grant, Milan Gembicky, Paul F. Richardson, Phil S. Baran","doi":"10.1038/s41929-025-01336-3","DOIUrl":"10.1038/s41929-025-01336-3","url":null,"abstract":"Tertiary nitroalkanes, as well as their reduced products, α-tertiary amines, play an essential role in drug discovery as either key synthetic precursors or final motifs in targeted molecules. Existing methods to prepare tertiary nitro compounds generally rely on polar-bond disconnections, in which strong bases or highly active electrophiles are needed. Here we report the development of an anomeric nitroamide-based reagent that enables selective metal-hydride hydrogen atom transfer-based Co-catalysed alkene hydronitration for the preparation of valuable tertiary nitro compounds. This mild, scalable reaction shows broad functional group tolerance. Its synthetic application is demonstrated via late-stage nitration of complex alkenes derived from drugs and natural products, and simplifying the synthesis of a rare naturally occurring nitro sugar. Simple access to isotopically labelled 15N-containing nitro compounds is also disclosed. The anomeric nitroamide reagent was deemed safe by energetic measurements and its reactivity rationalized based on X-ray crystallographic analysis. Synthetic methods to generate tertiary nitroalkanes are scarce. Now the cobalt-catalysed synthesis of tertiary nitro-containing compounds under mild conditions from easily available olefins is enabled by a nitro-transfer reagent containing an anomeric amide.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 5","pages":"457-464"},"PeriodicalIF":44.6,"publicationDate":"2025-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144104482","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

Dissolved Fe species enable a cooperative solid–molecular mechanism for the oxygen evolution reaction on NiFe-based catalysts 溶解的铁元素使镍铁基催化剂上的析氧反应具有协同的固-分子机制

IF 44.6 1区化学

Nature Catalysis Pub Date : 2025-05-20 DOI: 10.1038/s41929-025-01342-5

Chunguang Kuai, Liping Liu, Anyang Hu, Yan Zhang, Yuxin Zhang, Dawei Xia, Dennis Nordlund, Dimosthenis Sokaras, Donato Decarolis, Diego Gianolio, Hongliang Xin, Luxi Li, Feng Lin

{"title":"Dissolved Fe species enable a cooperative solid–molecular mechanism for the oxygen evolution reaction on NiFe-based catalysts","authors":"Chunguang Kuai, Liping Liu, Anyang Hu, Yan Zhang, Yuxin Zhang, Dawei Xia, Dennis Nordlund, Dimosthenis Sokaras, Donato Decarolis, Diego Gianolio, Hongliang Xin, Luxi Li, Feng Lin","doi":"10.1038/s41929-025-01342-5","DOIUrl":"10.1038/s41929-025-01342-5","url":null,"abstract":"The oxygen evolution reaction is a key process in many energy technologies, but improving its efficiency remains challenging due to the energy scaling relationships that limit the reaction kinetics on conventional single-active-site solid catalysts. Here we report a cooperative solid–molecular mechanism for oxygen evolution on NiFe-based hydroxide electrocatalysts. By identifying the critical interfacial species and understanding their dynamics, we find that molecular FeO42− species, derived from the dissolution of Fe from the solid catalyst, act as molecular co-catalysts that participate in the critical O–O bond-formation step along with solid sites. This synergistic mechanism, involving both solid and molecular active species, circumvents the typical scaling limitations observed for solid catalysts alone. Our findings reveal an unconventional solid–molecular mechanism that governs electrocatalysis at the solid–liquid interface and suggest a strategy for transcending scaling constraints through cooperative multi-site catalysis. NiFe-based catalysts are promising for water oxidation in alkaline electrolytes, but their dynamic structure under operation hinders the establishment of design principles for improved catalytic performance. Now a water oxidation mechanism on mixed NiFe hydroxide catalysts is proposed that involves dissolved FeO42− species acting as co-catalysts.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 6","pages":"523-535"},"PeriodicalIF":44.6,"publicationDate":"2025-05-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144097157","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

Organocatalytic regio- and stereoselective cyclopropanation of olefins 烯烃的有机催化区域选择性和立体选择性环丙烷化

IF 44.6 1区化学

Nature Catalysis Pub Date : 2025-05-16 DOI: 10.1038/s41929-025-01340-7

Chendan Zhu, Sayantani Das, Avishek Guin, Chandra Kanta De, Benjamin List

{"title":"Organocatalytic regio- and stereoselective cyclopropanation of olefins","authors":"Chendan Zhu, Sayantani Das, Avishek Guin, Chandra Kanta De, Benjamin List","doi":"10.1038/s41929-025-01340-7","DOIUrl":"10.1038/s41929-025-01340-7","url":null,"abstract":"As reactive intermediates and substructures of natural products and bioactive molecules, the smallest cyclic alkanes—cyclopropanes—are an attractive class of molecules for chemists. Arguably, the most general approach to their chemical synthesis involves the addition of metal carbenes to olefins. Whereas catalytic asymmetric cyclopropanations of electronically unbiased olefins with carbenoids have been reported using chiral metal complexes and engineered metalloenzymes, we now report a complementary, metal-free and highly enantioselective cyclopropanation of olefins with diazoalkanes, applying asymmetric counteranion-directed photoredox organocatalysis. We identify an ion pair featuring a thioxanthylium photoredox cation and a chiral imidodiphosphorimidate counteranion that catalyses highly enantioselective cyclopropanations of styrenes and aliphatic dienes with diazo compounds. Mechanistic investigations reveal a wavelength dependence of the enantioselectivity and suggest that the main catalytic pathway proceeds via olefin-derived radical cation intermediates. This metal-free, highly enantioselective organocatalytic approach complements previously reported methods for alkene manipulations. Transformations from carbenes to olefins have generally been realized with transition metal-catalysed enantioselective methods or artificial metalloenzymes. Here the authors apply asymmetric counteranion-directed photoredox organocatalysis for the highly enantioselective cyclopropanation of styrenes and aliphatic dienes.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 5","pages":"487-494"},"PeriodicalIF":44.6,"publicationDate":"2025-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.comhttps://www.nature.com/articles/s41929-025-01340-7.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144066183","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