Pub Date : 2024-05-02DOI: 10.1038/s41929-024-01170-z
Christopher Fröhlich, H. Adrian Bunzel, Karol Buda, Adrian J. Mulholland, Marc W. van der Kamp, Pål J. Johnsen, Hanna-Kirsti S. Leiros, Nobuhiko Tokuriki
{"title":"Author Correction: Epistasis arises from shifting the rate-limiting step during enzyme evolution of a β-lactamase","authors":"Christopher Fröhlich, H. Adrian Bunzel, Karol Buda, Adrian J. Mulholland, Marc W. van der Kamp, Pål J. Johnsen, Hanna-Kirsti S. Leiros, Nobuhiko Tokuriki","doi":"10.1038/s41929-024-01170-z","DOIUrl":"10.1038/s41929-024-01170-z","url":null,"abstract":"","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":null,"pages":null},"PeriodicalIF":37.8,"publicationDate":"2024-05-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41929-024-01170-z.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141019957","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}
Pub Date : 2024-04-30DOI: 10.1038/s41929-024-01138-z
Shao-Hua Xiang, Wei-Yi Ding, Yong-Bin Wang, Bin Tan
Atropisomeric architectures are increasingly encountered in modern materials and medicinally important compounds. More importantly, they are now a characteristic of broadly useful chiral ligands and organocatalysts. Over the past decade, substantial advancements have been made in enhancing the accessibility of major classes of atropisomers through the refinement of existing strategies and the introduction of contemporary concepts for catalytic atroposelective synthesis. This synthetic capability enables the expansion of chemical space and facilitates the preparation of valuable atropisomeric scaffolds. Here we review the state of the art in the asymmetric synthesis of atropisomers with the help of selected examples. Focus will be placed on the strategies that have emerged rapidly in recent years, and that are characterized by high versatility and modularity. Additionally, the incorporation of emerging synthetic tools and representative scaffolds are discussed, alongside future directions in this research domain. Atropisomerism is an expanding target of asymmetric catalysis. In this Review, recent advances in atroposelective synthesis under catalytic control are highlighted with a focus on general strategies that provide high versatility and modularity.
{"title":"Catalytic atroposelective synthesis","authors":"Shao-Hua Xiang, Wei-Yi Ding, Yong-Bin Wang, Bin Tan","doi":"10.1038/s41929-024-01138-z","DOIUrl":"10.1038/s41929-024-01138-z","url":null,"abstract":"Atropisomeric architectures are increasingly encountered in modern materials and medicinally important compounds. More importantly, they are now a characteristic of broadly useful chiral ligands and organocatalysts. Over the past decade, substantial advancements have been made in enhancing the accessibility of major classes of atropisomers through the refinement of existing strategies and the introduction of contemporary concepts for catalytic atroposelective synthesis. This synthetic capability enables the expansion of chemical space and facilitates the preparation of valuable atropisomeric scaffolds. Here we review the state of the art in the asymmetric synthesis of atropisomers with the help of selected examples. Focus will be placed on the strategies that have emerged rapidly in recent years, and that are characterized by high versatility and modularity. Additionally, the incorporation of emerging synthetic tools and representative scaffolds are discussed, alongside future directions in this research domain. Atropisomerism is an expanding target of asymmetric catalysis. In this Review, recent advances in atroposelective synthesis under catalytic control are highlighted with a focus on general strategies that provide high versatility and modularity.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":null,"pages":null},"PeriodicalIF":37.8,"publicationDate":"2024-04-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140814377","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}
Pub Date : 2024-04-29DOI: 10.1038/s41929-024-01153-0
Xia Hu, Iván Cheng-Sánchez, Wangqing Kong, Gary A. Molander, Cristina Nevado
The development of novel strategies to rapidly construct complex chiral molecules from readily available feedstocks is a long-term pursuit in the chemistry community. Radical-mediated alkene difunctionalizations represent an excellent platform towards this goal. However, asymmetric versions remain highly challenging, and more importantly, examples featuring simple hydrocarbons as reaction partners are elusive. Here we report an asymmetric three-component alkene dicarbofunctionalization capitalizing on the direct activation of C(sp3)–H bonds through the combination of photocatalysed hydrogen atom transfer and nickel catalysis. This protocol provides an efficient platform for installing two vicinal carbon–carbon bonds across alkenes in an atom-economic fashion, providing a wide array of high-value chiral α-aryl/alkenyl carbonyls and phosphonates, as well as 1,1-diarylalkanes from ubiquitous alkane, ether and alcohol feedstocks. This method exhibits operational simplicity, broad substrate scope and excellent regioselectivity, chemoselectivity and enantioselectivity. The compatibility with bioactive motifs and expedient synthesis of pharmaceutically relevant molecules highlight the synthetic potential of this protocol. Asymmetric versions of radical-mediated alkene difunctionalizations featuring hydrocarbon precursors are currently elusive. Here the authors report an asymmetric vicinal alkene dicarbofunctionalization based on the activation of C(sp3)–H bonds through the combination of photocatalysed hydrogen atom transfer and nickel catalysis.
{"title":"Nickel-catalysed enantioselective alkene dicarbofunctionalization enabled by photochemical aliphatic C–H bond activation","authors":"Xia Hu, Iván Cheng-Sánchez, Wangqing Kong, Gary A. Molander, Cristina Nevado","doi":"10.1038/s41929-024-01153-0","DOIUrl":"10.1038/s41929-024-01153-0","url":null,"abstract":"The development of novel strategies to rapidly construct complex chiral molecules from readily available feedstocks is a long-term pursuit in the chemistry community. Radical-mediated alkene difunctionalizations represent an excellent platform towards this goal. However, asymmetric versions remain highly challenging, and more importantly, examples featuring simple hydrocarbons as reaction partners are elusive. Here we report an asymmetric three-component alkene dicarbofunctionalization capitalizing on the direct activation of C(sp3)–H bonds through the combination of photocatalysed hydrogen atom transfer and nickel catalysis. This protocol provides an efficient platform for installing two vicinal carbon–carbon bonds across alkenes in an atom-economic fashion, providing a wide array of high-value chiral α-aryl/alkenyl carbonyls and phosphonates, as well as 1,1-diarylalkanes from ubiquitous alkane, ether and alcohol feedstocks. This method exhibits operational simplicity, broad substrate scope and excellent regioselectivity, chemoselectivity and enantioselectivity. The compatibility with bioactive motifs and expedient synthesis of pharmaceutically relevant molecules highlight the synthetic potential of this protocol. Asymmetric versions of radical-mediated alkene difunctionalizations featuring hydrocarbon precursors are currently elusive. Here the authors report an asymmetric vicinal alkene dicarbofunctionalization based on the activation of C(sp3)–H bonds through the combination of photocatalysed hydrogen atom transfer and nickel catalysis.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":null,"pages":null},"PeriodicalIF":42.8,"publicationDate":"2024-04-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41929-024-01153-0.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140808364","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}
Pub Date : 2024-04-26DOI: 10.1038/s41929-024-01159-8
Marçal Capdevila-Cortada
{"title":"Murder on the micropore","authors":"Marçal Capdevila-Cortada","doi":"10.1038/s41929-024-01159-8","DOIUrl":"10.1038/s41929-024-01159-8","url":null,"abstract":"","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":null,"pages":null},"PeriodicalIF":37.8,"publicationDate":"2024-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140651218","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}
Pub Date : 2024-04-26DOI: 10.1038/s41929-024-01139-y
Dongsoo Yang
Malonyl-CoA is one of the fundamental building blocks for the synthesis of industrially or pharmaceutically important chemicals, but its biosynthesis via the innate acetyl-CoA carboxylation pathway remains slow and inefficient. Now, an artificial non-carboxylative malonyl-CoA biosynthetic pathway has been developed, significantly enhancing malonyl-CoA supply by boosting carbon and energy efficiency while sidestepping the inhibitions by host cell regulations.
{"title":"Acetyl-CoA-independent malonyl-CoA biosynthesis","authors":"Dongsoo Yang","doi":"10.1038/s41929-024-01139-y","DOIUrl":"10.1038/s41929-024-01139-y","url":null,"abstract":"Malonyl-CoA is one of the fundamental building blocks for the synthesis of industrially or pharmaceutically important chemicals, but its biosynthesis via the innate acetyl-CoA carboxylation pathway remains slow and inefficient. Now, an artificial non-carboxylative malonyl-CoA biosynthetic pathway has been developed, significantly enhancing malonyl-CoA supply by boosting carbon and energy efficiency while sidestepping the inhibitions by host cell regulations.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":null,"pages":null},"PeriodicalIF":37.8,"publicationDate":"2024-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140651245","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}
Pub Date : 2024-04-26DOI: 10.1038/s41929-024-01151-2
Xun Guan, Yongchao Xie, Chong Liu
Hybrid systems that integrate synthetic materials with biological machinery offer opportunities for sustainable and efficient catalysis. However, the multidisciplinary and unique nature of the materials–biology interface requires researchers to draw insights from different fields. In this Perspective, using examples from the area of N2 and CO2 fixation, we provide a unified discussion of critical aspects of the material–microbe interface, simultaneously considering the requirements of physical and biological sciences that have a tangible impact on the performance of biohybrids. We first discuss the figures of merit and caveats for the evaluation of catalytic performance. Then, we reflect on the interactions and potential synergies at the materials–biology interface, as well as the challenges and opportunities for a deepened fundamental understanding of abiotic–biotic catalysis. Material–microbe hybrids represent an interesting class of catalyst with potential for high energy efficiency and product selectivity. In this Perspective the authors discuss some of the difficulties in understanding these interdisciplinary systems and the attempts to unify the approaches taken by different research communities to further the field.
将合成材料与生物机械相结合的混合系统为可持续高效催化提供了机会。然而，材料-生物界面的多学科性和独特性要求研究人员从不同领域汲取见解。在本《视角》中，我们以 N2 和 CO2 固定领域为例，对材料-微生物界面的关键方面进行了统一讨论，同时考虑了对生物混合体性能有切实影响的物理科学和生物科学的要求。我们首先讨论了评估催化性能的优点和注意事项。然后，我们思考了材料-生物学界面的相互作用和潜在协同作用，以及加深对非生物-生物催化的基本理解所面临的挑战和机遇。
{"title":"Performance evaluation and multidisciplinary analysis of catalytic fixation reactions by material–microbe hybrids","authors":"Xun Guan, Yongchao Xie, Chong Liu","doi":"10.1038/s41929-024-01151-2","DOIUrl":"10.1038/s41929-024-01151-2","url":null,"abstract":"Hybrid systems that integrate synthetic materials with biological machinery offer opportunities for sustainable and efficient catalysis. However, the multidisciplinary and unique nature of the materials–biology interface requires researchers to draw insights from different fields. In this Perspective, using examples from the area of N2 and CO2 fixation, we provide a unified discussion of critical aspects of the material–microbe interface, simultaneously considering the requirements of physical and biological sciences that have a tangible impact on the performance of biohybrids. We first discuss the figures of merit and caveats for the evaluation of catalytic performance. Then, we reflect on the interactions and potential synergies at the materials–biology interface, as well as the challenges and opportunities for a deepened fundamental understanding of abiotic–biotic catalysis. Material–microbe hybrids represent an interesting class of catalyst with potential for high energy efficiency and product selectivity. In this Perspective the authors discuss some of the difficulties in understanding these interdisciplinary systems and the attempts to unify the approaches taken by different research communities to further the field.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":null,"pages":null},"PeriodicalIF":37.8,"publicationDate":"2024-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140648710","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}
Pub Date : 2024-04-26DOI: 10.1038/s41929-024-01145-0
Shinya Fushinobu
Gut microbes have enzymes that break down the heavily glycosylated mucin protein of host animals, but known enzymes recognize only one glycan chain. Now, bioinformatic exploration has uncovered a family of mucinases that targets dense sugar residues.
{"title":"Taking a walk to find new mucinases","authors":"Shinya Fushinobu","doi":"10.1038/s41929-024-01145-0","DOIUrl":"10.1038/s41929-024-01145-0","url":null,"abstract":"Gut microbes have enzymes that break down the heavily glycosylated mucin protein of host animals, but known enzymes recognize only one glycan chain. Now, bioinformatic exploration has uncovered a family of mucinases that targets dense sugar residues.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":null,"pages":null},"PeriodicalIF":37.8,"publicationDate":"2024-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140651256","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}
Pub Date : 2024-04-26DOI: 10.1038/s41929-024-01146-z
Haisong Feng, Xin Zhang
Ethylene, despite being a cornerstone of the modern petrochemical industry, continues to pose challenges during its production. Now, a dual single-atom catalyst design emerges as a remarkable solution for the efficient semi-hydrogenation of acetylene.
{"title":"Tailored for semi-hydrogenation","authors":"Haisong Feng, Xin Zhang","doi":"10.1038/s41929-024-01146-z","DOIUrl":"10.1038/s41929-024-01146-z","url":null,"abstract":"Ethylene, despite being a cornerstone of the modern petrochemical industry, continues to pose challenges during its production. Now, a dual single-atom catalyst design emerges as a remarkable solution for the efficient semi-hydrogenation of acetylene.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":null,"pages":null},"PeriodicalIF":37.8,"publicationDate":"2024-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140651261","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}
京公网安备 11010802042870号
京ICP备2023020795号-1
扫码关注我们
求助内容：
应助结果提醒方式：