ACS Catalysis 最新文献

Glutathione S-Transferase Mediated Epoxide Conversion: Functional and Structural Properties of an Enantioselective Catalyst 谷胱甘肽s -转移酶介导的环氧化物转化：对映选择性催化剂的功能和结构性质

IF 12.9 1区化学

ACS Catalysis Pub Date : 2025-07-07 DOI: 10.1021/acscatal.5c02430

Melody Haarmann, Max Scholz, Anna C. Lienkamp, Jan Burnik, Bo Højen Justesen, Jens Reiners, Artur Maier, Daniel Eggerichs, Kai Vocke, Sander H. J. Smits, Thomas Günther Pomorski, Eckhard Hofmann, Dirk Tischler

{"title":"Glutathione S-Transferase Mediated Epoxide Conversion: Functional and Structural Properties of an Enantioselective Catalyst","authors":"Melody Haarmann, Max Scholz, Anna C. Lienkamp, Jan Burnik, Bo Højen Justesen, Jens Reiners, Artur Maier, Daniel Eggerichs, Kai Vocke, Sander H. J. Smits, Thomas Günther Pomorski, Eckhard Hofmann, Dirk Tischler","doi":"10.1021/acscatal.5c02430","DOIUrl":"https://doi.org/10.1021/acscatal.5c02430","url":null,"abstract":"Styrene is a naturally occurring but mainly anthropogenically produced aromatic compound. It is degraded via different routes in nature but often activated to styrene oxide, predominantly to its (S)-enantiomer. Hence, downstream enzymes should have regio- and enantio-preference. We have now demonstrated the enantioselectivity for a previously unknown class of bacterial glutathione S-transferases (GST) using both structural and kinetic approaches. Four actinobacterial GSTs were tested for their activity and selectivity. The most promising enzyme, GrStyI from Gordonia rubripertincta CWB2, was further investigated regarding its enantioselectivity and unique structure. GrStyI occurs as a homodimer and accepts (S)-styrene oxide (76 ± 3 μmol min–1 mg–1). It appears to be promiscuous in terms of structurally related epoxides and efficient for kinetic racemic resolution, providing a means for simple access toward (R)-epoxides, as we show in this study. We propose the presence of enantioselective GSTs in actinobacteria, forming the class of Actino-like GSTs.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"85 1","pages":""},"PeriodicalIF":12.9,"publicationDate":"2025-07-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144568883","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

Enantioselective Copper-Catalyzed Desymmetric Olefination via the Boron-Wittig Reaction 铜催化硼-维蒂格反应的对映选择性不对称烯烃反应

IF 12.9 1区化学

ACS Catalysis Pub Date : 2025-07-07 DOI: 10.1021/acscatal.5c02755

Dongzhen Xu, Weike Li, Wenze Shi, Xihong Wang, Min Wang, Jian Liao

引用次数: 0

Acid-Catalyzed, Three-Component, Spontaneous Cascades of 1,3-Butadiynyl Propargylic Alcohols as a Route to Phthalan Derivatives 酸催化，三组分，自发级联1,3-丁二炔丙炔醇合成酞菁衍生物的途径

IF 12.9 1区化学

ACS Catalysis Pub Date : 2025-07-06 DOI: 10.1021/acscatal.5c03571

Jingyang Shi, Thomas R. Hoye

引用次数: 0

Advances in Physical Mixture Catalysts as a Heterogeneous Catalytic Strategy: A Review 物理混合催化剂作为一种多相催化策略的研究进展

IF 12.9 1区化学

ACS Catalysis Pub Date : 2025-07-05 DOI: 10.1021/acscatal.5c03486

Xiaoyang Jerry Huang, Guihua Liu, Ying Tao, Liang Zhao, Jian Yang, Rena Oh, Shi-Gang Sun

{"title":"Advances in Physical Mixture Catalysts as a Heterogeneous Catalytic Strategy: A Review","authors":"Xiaoyang Jerry Huang, Guihua Liu, Ying Tao, Liang Zhao, Jian Yang, Rena Oh, Shi-Gang Sun","doi":"10.1021/acscatal.5c03486","DOIUrl":"https://doi.org/10.1021/acscatal.5c03486","url":null,"abstract":"Metal alloys are widely recognized for their high catalytic activity in the field of heterogeneous catalysis. This enhanced performance arises from various alloying effects between the constituent atoms within multimetallic particles. Recently, our research group discovered that physically separating metals from their alloyed state and forming a physical mixture can further enhance catalytic performance across a range of reactions, including thermochemical and electrochemical processes. In this catalytic system, each type of metal serves as an active site for a distinct subreaction. These subreactions are effectively coupled through the intimate contact between catalytic components, which facilitates the transfer of reaction intermediates across the carbon support. In this review, we discuss recent advances in understanding this catalytic effect, with special interest in thermocatalysis and electrocatalysis. While significant progress has been made in improving reaction rates, future research should also focus on enhancing product selectivity and expanding the application of this approach to photochemical reactions.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"10 1","pages":""},"PeriodicalIF":12.9,"publicationDate":"2025-07-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144568985","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

Computationally Guided Development of an Alkene Aminocarboxylation with CO2: Synthesis of a β-Amino Acid Derivative 以计算为导向的烯烃氨基羧化反应的发展：β-氨基酸衍生物的合成

IF 12.9 1区化学

ACS Catalysis Pub Date : 2025-07-04 DOI: 10.1021/acscatal.5c03580

Wataru Kanna, Yu Harabuchi, Kosaku Tanaka, III, Hiroki Hayashi, Hideaki Takano, Tomoki Kozuka, Hiroto Sakurai, Nobuyuki Mase, Satoshi Maeda, Tsuyoshi Mita

{"title":"Computationally Guided Development of an Alkene Aminocarboxylation with CO2: Synthesis of a β-Amino Acid Derivative","authors":"Wataru Kanna, Yu Harabuchi, Kosaku Tanaka, III, Hiroki Hayashi, Hideaki Takano, Tomoki Kozuka, Hiroto Sakurai, Nobuyuki Mase, Satoshi Maeda, Tsuyoshi Mita","doi":"10.1021/acscatal.5c03580","DOIUrl":"https://doi.org/10.1021/acscatal.5c03580","url":null,"abstract":"β-Amino acids are important structural motifs in synthetic organic chemistry owing to their applications as components in artificial peptides, which are intensively studied in pharmaceutical science. While various strategies exist for synthesizing α- and γ-amino acids from CO2 via α-amino carbanion or α-aminoalkyl radical intermediates, direct and concise routes to β-amino acids remain rare. Herein, we report the computationally guided development of a photoredox-catalyzed aminocarboxylation of an aminoalkene with CO2, affording a β-amino acid derivative under mild conditions. Although the demonstrated scope is currently limited, this transformation showcases a mechanistically distinct reactivity pattern enabled by photoredox catalysis. The reaction was inspired by our previous multistate reaction path network explored for Knowles’ hydroamination, where we found that a seam of crossing (SX) point for the potential energy surface involving a CH3OH molecule facilitates product formation via proton-coupled electron transfer. Upon substituting CH3OH with CO2, the corresponding SX calculations indicated that the energetically concerted reduction–carboxylation mechanism is feasible. Indeed, cyclic β-amino acids were obtained from amino alkenes using [Ir(ppy)2(dtbbpy)]PF6 as a photoredox catalyst under irradiation with blue LEDs (440 nm). The developed photoreaction was successfully applied to a gas–liquid flow system under CO2 pressure (1.0 MPa), in which the blue LEDs irradiated the tube line (total volume: 4.6 mL) for merely 3.2 min to afford the desired β-amino acids in good yield.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"31 1","pages":""},"PeriodicalIF":12.9,"publicationDate":"2025-07-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144568886","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

IF 11.3 1区化学