Chem Catalysis最新文献

SubTuner leverages physics-based modeling to complement AI in enzyme engineering toward non-native substrates

IF 9.4

Chem Catalysis Pub Date : 2025-03-28 DOI: 10.1016/j.checat.2025.101334

Qianzhen Shao, Asher C. Hollenbeak, Yaoyukun Jiang, Xinchun Ran, Brian O. Bachmann, Zhongyue J. Yang

{"title":"SubTuner leverages physics-based modeling to complement AI in enzyme engineering toward non-native substrates","authors":"Qianzhen Shao, Asher C. Hollenbeak, Yaoyukun Jiang, Xinchun Ran, Brian O. Bachmann, Zhongyue J. Yang","doi":"10.1016/j.checat.2025.101334","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101334","url":null,"abstract":"We developed SubTuner, a physics-based computational tool that tackles the challenge of identifying enzyme mutants with enhanced activity for specified non-native substrates. To test the performance of SubTuner, we designed three tasks, all aiming to identify beneficial anion methyltransferase mutants for synthesis of non-native S-adenosyl-L-methionine analogs: first, in the conversion of ethyl iodide from a pool of 190 Arabidopsis thaliana Harmless to Ozone Layer 1 (AtHOL1) single-point mutants for an initial test of accuracy and speed; second, of ethyl, n-propyl, cyclopropylmethyl, and phenethyl iodides from a pool of 600 Aspergillus clavatus methyltransferase multi-point mutants for a test of generalizability; and, eventually, of bulkier substrates for AtHOL1 combined with experimental characterization for a test of a priori predictivity. All tests demonstrated SubTuner’s ability to accelerate enzyme engineering for non-native substrates, superior to existing bioinformatics and machine-learning-based tools. SubTuner, with its physical hypothesis, quantitative accuracy, and mechanism-informing ability, holds significant potential to aid enzyme engineering for substrate scope expansion.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"36 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723935","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Enantioselective palladium-catalyzed α-arylation of primary alkylamines

IF 9.4

Chem Catalysis Pub Date : 2025-03-28 DOI: 10.1016/j.checat.2025.101331

Zoutao Wang, Shuai Guo, Ziyang Shen, Ran Wei, Ruijie Jiang, Guodu Liu, Qinghai Zhou, Kang Du, Wenjun Tang

引用次数: 0

Recent progress in understanding mechanism of electrochemical oxygen evolution reaction via operando/in situ characterizations

IF 9.4

Chem Catalysis Pub Date : 2025-03-28 DOI: 10.1016/j.checat.2025.101332

Rashid Mehmood, Fuxiang Zhang

{"title":"Recent progress in understanding mechanism of electrochemical oxygen evolution reaction via operando/in situ characterizations","authors":"Rashid Mehmood, Fuxiang Zhang","doi":"10.1016/j.checat.2025.101332","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101332","url":null,"abstract":"Understanding the mechanism of the oxygen evolution reaction (OER) represents a bottleneck in designing efficient energy storage schemes based on water splitting. However, identifying the mechanism experimentally has proven a grand challenge. This could be due to the diverse nature of OER intermediates. Recent progress in operando/in situ characterizations has provided an unprecedented understanding of the OER mechanisms concerning active site identification, as well as other OER mechanisms. On this basis, we offer a comprehensive discussion on experimental evidence for identifying OER intermediates experimentally, aligning them with theoretical calculations in designing future green energy systems. Finally, some perspectives that are anticipated to be beneficial to addressing the current challenges in operando/in situ monitoring of active site identification and understanding of the underlying mechanisms of OER electrocatalysts are presented. This review aims to provide new insights into the rational design of OER catalytic materials and offers a complete understanding of OER mechanisms.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"64 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723934","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Stretchable asymmetric dual-atom Cu(I) electrocatalyst for enhanced CO2 reduction to C2+ products

IF 9.4

Chem Catalysis Pub Date : 2025-03-24 DOI: 10.1016/j.checat.2025.101327

Ran Bu, Shuaiqiang Jia, YuHou Pei, Danyun Xu, Di Li, Qidong Ruan, Yuting Liu, Pengfei Mu, Enqing Gao, Yingying Lu, Bing Zhang

{"title":"Stretchable asymmetric dual-atom Cu(I) electrocatalyst for enhanced CO2 reduction to C2+ products","authors":"Ran Bu, Shuaiqiang Jia, YuHou Pei, Danyun Xu, Di Li, Qidong Ruan, Yuting Liu, Pengfei Mu, Enqing Gao, Yingying Lu, Bing Zhang","doi":"10.1016/j.checat.2025.101327","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101327","url":null,"abstract":"Constructing precise catalytic sites and local microenvironments to achieve electrochemical CO2 conversion to valuable C2+ products remains a great challenge. Here, a porous crystalline covalent organic framework (COF) containing Br-bridged dual single-atom Cu(I) sites with an asymmetric coordination environment was rationally designed and confirmed by combining single-crystal X-ray diffraction and X-ray absorption fine structure analyses. The as-synthesized COF-based single-atom Cu catalyst exhibits exceptional performance in the electrochemical CO2 reduction reaction to C2+ products, which surpasses that of most previously reported single-atom catalysts with defined coordination structures. Operando Raman spectroscopy, theoretical calculations, and control experiments were employed to verify the mechanism behind the effectiveness of the catalyst. These investigations suggest that the flexible, asymmetrically coordinated dual-atom Cu(I) sites can lower the energy barrier for generating ∗CO and ∗COCHO intermediates, thereby promoting the formation of C–C bonds necessary for C2+ products.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"15 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143677973","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Strain relaxation enhances ammonia electrosynthesis from nitrate on Cu/CuAu core/shell nanocrystals with ordered intermetallic layers

IF 9.4

Chem Catalysis Pub Date : 2025-03-24 DOI: 10.1016/j.checat.2025.101328

Qiang Gao, Bingqing Yao, Yuanqi Liu, Lei Shi, Zihao Yan, Libang Xu, Qian He, Huiyuan Zhu

{"title":"Strain relaxation enhances ammonia electrosynthesis from nitrate on Cu/CuAu core/shell nanocrystals with ordered intermetallic layers","authors":"Qiang Gao, Bingqing Yao, Yuanqi Liu, Lei Shi, Zihao Yan, Libang Xu, Qian He, Huiyuan Zhu","doi":"10.1016/j.checat.2025.101328","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101328","url":null,"abstract":"Recycling ammonia (NH3) via the electrocatalytic nitrate reduction reaction (NO3RR) offers a sustainable, energy-efficient solution for closing the nitrogen cycle while simultaneously treating nitrate-rich wastewater. In this work, we synthesized core/shell Cu/CuAu nanocubes with precisely controlled ordered intermetallic layers using a facile seed-mediated method. The compressive surface strain of the nanocrystals was finely regulated by adjusting the layers of the CuAu shell. Specifically, the strain-relaxed Cu/CuAu catalysts exhibit high NO3RR performance for NH3 production, achieving a Faradic efficiency of 89.9% at −0.5 V vs. the reversible hydrogen electrode (RHE) and an exceedingly high yield rate of 11.3 mol h−1 g−1 at −0.6 V vs. RHE. Furthermore, Cu/CuAu catalysts show catalytic stability over 10 consecutive cycles and 12-h electrolysis. This atomic-level control of thickness allows precise tuning of the intrinsic strain to optimize catalytic reactivity, offering a promising strategy to enhance the performance of electrocatalytic ammonia synthesis.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"16 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143677974","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Cation-coupled electron transfer in the oxygen reduction reaction and beyond

IF 9.4

Chem Catalysis Pub Date : 2025-03-20 DOI: 10.1016/j.checat.2025.101304

Yifei Xu, Bingjun Xu

引用次数: 0

Scaling solar hydrogen peroxide

IF 9.4

Chem Catalysis Pub Date : 2025-03-20 DOI: 10.1016/j.checat.2025.101333

Emily H. Edwards

引用次数: 0

A Pt-Fe-Pt heterotrimer for selective hydrogenation of crotonaldehyde

IF 9.4

Chem Catalysis Pub Date : 2025-03-20 DOI: 10.1016/j.checat.2025.101301

Duc Nam Do, Ngoc Thanh Ngan Thai, Bin Wang

引用次数: 0

Ligands-regulated ∗CO adsorption on two-dimensional covalent organic framework promotes selective electrochemical CO2 conversion

IF 9.4

Chem Catalysis Pub Date : 2025-03-19 DOI: 10.1016/j.checat.2025.101325

Yuluo Shen, Jiyuan Liu, Guoshuai Shi, Chunlei Yang, Tingyu Lu, Mingwei Chang, Yijie Wu, Shuzhou Li, Dong-Jin Qian, Liming Zhang

{"title":"Ligands-regulated ∗CO adsorption on two-dimensional covalent organic framework promotes selective electrochemical CO2 conversion","authors":"Yuluo Shen, Jiyuan Liu, Guoshuai Shi, Chunlei Yang, Tingyu Lu, Mingwei Chang, Yijie Wu, Shuzhou Li, Dong-Jin Qian, Liming Zhang","doi":"10.1016/j.checat.2025.101325","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101325","url":null,"abstract":"Manipulating the adsorption/desorption of intermediates at active sites offers a promising strategy to direct specific electrocatalytic pathways. In high overpotential regimes, the desorption of ∗CO from active sites is a major limitation in electrochemical CO2-to-CO conversion, emphasizing the need to control ∗CO adsorption strength. Here, we report a series of well-defined amide-linked covalent organic frameworks (COFs) featuring alternating tetraaminophenylporphyrin and tetracarboxyphenylporphyrin building blocks, with M1 and M2 sites (M1/M2 = Co, Fe). Electrochemical tests and computational models reveal that the polar ligand framework plays a key role in regulating ∗CO adsorption, a conclusion supported by operando spectroelectrochemical measurements. Theoretical calculations attribute this regulation to the differing <math><mrow is=\"true\"><msub is=\"true\"><mi is=\"true\" mathvariant=\"normal\">d</mi><msup is=\"true\"><mi is=\"true\" mathvariant=\"normal\">z</mi><mn is=\"true\">2</mn></msup></msub></mrow></math> band centers of the transition metals, driven by intra-layer charge transfer from polar amine bonds. This work underscores the importance of polar ligands in optimizing intermediate adsorption and enhancing CO2 transformation efficiency.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"70 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143653996","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Dynamic kinetic resolution and dynamic kinetic asymmetric transformation of atropisomeric biaryls

IF 9.4

Chem Catalysis Pub Date : 2025-03-18 DOI: 10.1016/j.checat.2025.101329

Jie Zhang, Xuanzhu Huo, Yidan Liu, Can Zhu

引用次数: 0