Nature Catalysis最新文献_第10页

Organocatalytic asymmetric α-C–H functionalization of alkyl amines 烷基胺的有机催化不对称 α-C-H 功能化

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-10-03 DOI: 10.1038/s41929-024-01230-4

Tianran Deng, Xiang-Lei Han, Yang Yu, Cheng Cheng, Xiangyuan Liu, Yuhong Gao, Keqiang Wu, Zhenghua Li, Jisheng Luo, Li Deng

{"title":"Organocatalytic asymmetric α-C–H functionalization of alkyl amines","authors":"Tianran Deng, Xiang-Lei Han, Yang Yu, Cheng Cheng, Xiangyuan Liu, Yuhong Gao, Keqiang Wu, Zhenghua Li, Jisheng Luo, Li Deng","doi":"10.1038/s41929-024-01230-4","DOIUrl":"10.1038/s41929-024-01230-4","url":null,"abstract":"Catalytic enantioselective α-C–H functionalization of widely available achiral alkyl amines could provide an ideal synthetic approach towards chiral amines. However, the inert nature of the α-C–H of alkyl amines renders their activation as carbanionic nucleophiles for catalytic asymmetric reactions an important yet unmet challenge. Here we describe how N-arylidene-protected alkyl amines could be activated as carbanions for asymmetric conjugate addition and the Mannich reaction. These results represent an intriguing and generally useful approach to the synthesis of chiral α,α-dialkyl amines. More importantly, they highlight the enormous potential of N-arylidene-protected amines as readily available and widely applicable synthons for the asymmetric synthesis of chiral amines. The catalytic activation of alkyl amines as α-nitrogen carbanions is challenging. Now the activation of N-arylidene-protected alkyl amines as carbanions by chiral ammonium organocatalysis for asymmetric conjugate addition and the Mannich reaction is reported, affording chiral α,α-dialkyl amines.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 10","pages":"1076-1085"},"PeriodicalIF":42.8,"publicationDate":"2024-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142368994","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

Author Correction: Localized thermal levering events drive spontaneous kinetic oscillations during CO oxidation on Rh/Al2O3 作者更正：局部热杠杆事件驱动 Rh/Al2O3 上 CO 氧化过程中的自发动力学振荡

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-10-03 DOI: 10.1038/s41929-024-01240-2

Donato Decarolis, Monik Panchal, Matthew Quesne, Khaled Mohammed, Shaojun Xu, Mark Isaacs, Adam H. Clark, Luke L. Keenan, Takuo Wakisaka, Kohei Kusada, Hiroshi Kitagawa, C. Richard A. Catlow, Emma K. Gibson, Alexandre Goguet, Peter P. Wells

引用次数: 0

Directed evolution of a highly efficient TNA polymerase achieved by homologous recombination 通过同源重组实现高效 TNA 聚合酶的定向进化

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-10-01 DOI: 10.1038/s41929-024-01233-1

Victoria A. Maola, Eric J. Yik, Mohammad Hajjar, Joy J. Lee, Manuel J. Holguin, Riley N. Quijano, Kalvin K. Nguyen, Katherine L. Ho, Jenny V. Medina, Nicholas Chim, John C. Chaput

{"title":"Directed evolution of a highly efficient TNA polymerase achieved by homologous recombination","authors":"Victoria A. Maola, Eric J. Yik, Mohammad Hajjar, Joy J. Lee, Manuel J. Holguin, Riley N. Quijano, Kalvin K. Nguyen, Katherine L. Ho, Jenny V. Medina, Nicholas Chim, John C. Chaput","doi":"10.1038/s41929-024-01233-1","DOIUrl":"10.1038/s41929-024-01233-1","url":null,"abstract":"Reprogramming DNA polymerases to synthesize xeno-nucleic acids (XNAs) is an important challenge that tests current enzyme engineering tools. Here we describe an evolutionary campaign aimed at generating an XNA polymerase that can efficiently make α-l-threofuranosyl nucleic acid (TNA)—an artificial genetic polymer that is recalcitrant to nucleases and resistant to acid-mediated degradation. Starting from a homologous recombination library, iterative cycles of selection were performed to traverse the fitness landscape in search of neutral mutations with increased evolutionary potential. Subsequent directed evolution of focused mutagenic libraries yielded 10–92, a newly engineered TNA polymerase that functions with a catalytic rate of ∼1 nt s−1 and >99% fidelity. A crystal structure of the closed ternary complex reveals the degree of structural change required to remodel the active site pocket for improved TNA synthesis activity. Together, these data demonstrate the importance of recombination as a strategy for evolving XNA polymerases with considerable practical value for biotechnology and medicine. The catalytic power of DNA polymerases for artificial genetic polymer (XNA) synthesis remains underdeveloped. Now, the evolution and structure of an α-l-threofuranosyl nucleic acid polymerase is described that achieves XNA synthesis with ∼1 nt s−1 and >99% template-copying fidelity.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 11","pages":"1173-1185"},"PeriodicalIF":42.8,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142330403","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

Step bunching instability and its effects in electrocatalysis on platinum surfaces 铂表面阶跃束化不稳定性及其对电催化的影响

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-09-30 DOI: 10.1038/s41929-024-01232-2

Francesc Valls Mascaró, Marc T. M. Koper, Marcel J. Rost

{"title":"Step bunching instability and its effects in electrocatalysis on platinum surfaces","authors":"Francesc Valls Mascaró, Marc T. M. Koper, Marcel J. Rost","doi":"10.1038/s41929-024-01232-2","DOIUrl":"10.1038/s41929-024-01232-2","url":null,"abstract":"The atomic-scale surface structure plays a major role in the electrochemical behaviour of a catalyst. The electrocatalytic activity towards many relevant reactions, such as the oxygen reduction reaction on platinum, exhibits a linear dependency with the number of steps until this linear scaling breaks down at high step densities. Here we show, using Pt(111)-vicinal surfaces and in situ electrochemical scanning tunnelling microscopy, that this anomalous behaviour at high step densities has a structural origin and is attributed to the bunching of closely spaced steps. While Pt(554) presents parallel single steps and terrace widths that correspond to its nominal, expected value, most steps on Pt(553) are bunched. Our findings challenge the common assumption in electrochemistry that all stepped surfaces are composed of homogeneously spaced steps of monoatomic height and can successfully explain the anomalous trends documented in the literature linking step density to both activity and potential of zero total charge. The electrocatalytic activity of metal catalysts commonly exhibits a positive linear correlation with the presence of steps, but this dependency breaks down for Pt catalysts with high step densities. Now, using in situ electrochemical scanning tunnelling microscopy, it is shown that this is due to the bunching of closely spaced steps, forming double and triple steps.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 11","pages":"1165-1172"},"PeriodicalIF":42.8,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142329493","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

Without that crystalline touch 没有那晶莹剔透的触感

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-09-24 DOI: 10.1038/s41929-024-01222-4

Xiaofei Guan

引用次数: 0

Deciphering electrochemical methanol production 解密电化学甲醇生产

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-09-24 DOI: 10.1038/s41929-024-01224-2

Stefan Ringe

引用次数: 0

Metallaphotoredox catalysis for sp3 C–H functionalizations through single-electron transfer 通过单电子转移实现 sp3 C-H 功能化的金属光氧催化

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-09-24 DOI: 10.1038/s41929-024-01215-3

Jingchang Zhang, Magnus Rueping

{"title":"Metallaphotoredox catalysis for sp3 C–H functionalizations through single-electron transfer","authors":"Jingchang Zhang, Magnus Rueping","doi":"10.1038/s41929-024-01215-3","DOIUrl":"10.1038/s41929-024-01215-3","url":null,"abstract":"Metallaphotoredox catalysis merging photocatalysis and transition metal catalysis is now the most efficient platform for sp3 C–H functionalizations due to its very efficient activation and transformation capability. In such a process, photocatalysis is usually in charge of C–H bond activation to generate an sp3-hybridized carbon-centred radical, whereas transition metal catalysis is in charge of the subsequent transformation of this radical. Here we review advances in sp3 C–H functionalizations under matallaphotoredox catalysis via photocatalytic single-electron transfer mechanisms as opposed to hydrogen atom transfer processes. The delineation of these advancements is initially organized according to distinct sp3 C–H bonds and subsequently categorized by various transition metal catalytic systems. We encompass a thorough exploration of diverse metallaphotoredox catalysis strategies, along with their synthetic applications and mechanisms. Similarities and differences between these strategies are described to inspire new reaction designs, thus promoting further development of this field. The merger of photocatalysis and transition metal catalysis has broadened the scope of chemical reactivity in organic synthesis. This Review provides an overview of the use of metallaphotoredox catalysis for sp3 C–H functionalizations that occur via single-electron, rather than hydrogen atom transfer.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 9","pages":"963-976"},"PeriodicalIF":42.8,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142313979","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

Solid electrolyte reactor for nitrate-to-ammonia 硝酸制氨固体电解质反应器

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-09-24 DOI: 10.1038/s41929-024-01223-3

Yuting Wang, Bin Zhang

引用次数: 0

Unlocking C–C cleavage in the electrochemical toolbox 打开电化学工具箱中的 C-C 裂解功能

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-09-24 DOI: 10.1038/s41929-024-01217-1

Nikolay Kornienko

引用次数: 0

Carbon conversion on biophotonic leaf 生物光子叶片上的碳转化