Chem Catalysis最新文献

Hinge loop reconstruction facilitates hydride transfer in Baeyer-Villiger monooxygenases 铰链环的重建促进了Baeyer-Villiger单加氧酶中的氢化物转移

IF 9.4

Chem Catalysis Pub Date : 2025-04-25 DOI: 10.1016/j.checat.2025.101364

Q. Geng, C.D. Zhou, Y.C. Zheng, F. Liu, Q. Chen, Z.J. Zhang, X.D. Kong, Z.K. Zhao, J.H. Xu, H.L. Yu

{"title":"Hinge loop reconstruction facilitates hydride transfer in Baeyer-Villiger monooxygenases","authors":"Q. Geng, C.D. Zhou, Y.C. Zheng, F. Liu, Q. Chen, Z.J. Zhang, X.D. Kong, Z.K. Zhao, J.H. Xu, H.L. Yu","doi":"10.1016/j.checat.2025.101364","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101364","url":null,"abstract":"To speed up biocatalytic redox reactions that use nicotinamide cofactors, previous researchers reshaped the cofactor-binding pocket, but this study focuses on the modification of a hinge loop outside the active site. This loop connects the FAD- and NADP-binding domains of AcPSMO (Acinetobacter calcoaceticus prazole sulfide monooxygenase). One penta-site mutant increased the catalytic efficiency with NADPH 87.5-fold more than the wild type, and another penta-site mutant increased the catalytic efficiency with NADH 12.9-fold more than the L143P mutant (the wild type was undetectable). These AcPSMO mutants also accepted two previously unreactive nicotinamide cofactor biomimetics as hydride donors. X-ray crystal structures and molecular dynamics simulations reveal that these substitutions move the bound NAD(P)H and FAD closer to one another. Introducing similar mutations in several other Baeyer-Villiger monooxygenases (BVMOs) also enhanced their catalytic activity. Thus, hinge-loop engineering is an effective alternative strategy to improve the reactivity of nicotinamide cofactors in BVMOs.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"258 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872121","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

Direct ammonia protonic ceramic fuel cells through heterogeneous interfaces engineering 基于异质界面工程的直接氨质子陶瓷燃料电池

IF 9.4

Chem Catalysis Pub Date : 2025-04-25 DOI: 10.1016/j.checat.2025.101365

Zuoqing Liu, Minghao Tao, Ming Xiao, Junbiao Li, Ruijia Xu, Bin Chen, Tao Li, Guangming Yang, Yuan Zhang, Nai Shi, Ran Ran, Wei Wang, Wei Zhou, Zongping Shao

{"title":"Direct ammonia protonic ceramic fuel cells through heterogeneous interfaces engineering","authors":"Zuoqing Liu, Minghao Tao, Ming Xiao, Junbiao Li, Ruijia Xu, Bin Chen, Tao Li, Guangming Yang, Yuan Zhang, Nai Shi, Ran Ran, Wei Wang, Wei Zhou, Zongping Shao","doi":"10.1016/j.checat.2025.101365","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101365","url":null,"abstract":"Ammonia, as an ideal carbon-free hydrogen carrier, enables direct application in protonic ceramic fuel cells while bypassing energy-intensive hydrogen regeneration. However, conventional Ni-based anodes for direct ammonia protonic ceramic fuel cells (DA-PCFCs) suffer from weak interfacial coupling and structural instability. Herein, we report a strategy of anodic heterogeneous engineering to build a strongly coupled Ni-BaZr0.1Ce0.7Y0.1Yb0.1O3-δ interface combined with a Cs2O-decorated Ru catalyst for surface modification. This design enhances ammonia decomposition by providing a highly interconnected network that facilitates efficient proton conduction and electron transfer, while the Ru catalyst introduces abundant active sites with superior ammonia adsorption capacity. The cell delivers a peak power density of 1.01 W cm−2 at 650°C and maintains 98.1% of its initial ammonia decomposition activity after 200 h at 500°C of operation. By overcoming the bottlenecks of DA-PCFCs, this study paves the way for their practical application in carbon-neutral energy systems.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"1 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872162","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

Electroreductively driven C–H functionalization of arenes 芳烃电还原驱动的碳氢官能化反应

IF 9.4

Chem Catalysis Pub Date : 2025-04-24 DOI: 10.1016/j.checat.2025.101359

Pengfei Xie, Anzai Shi, Youai Qiu

引用次数: 0

Peptide catalysis: Trends and opportunities 肽催化：趋势与机遇

IF 9.4

Chem Catalysis Pub Date : 2025-04-21 DOI: 10.1016/j.checat.2025.101339

Tom H.R. Kuster, Tobias Schnitzer

引用次数: 0

Tandem catalytic strategy for converting biogas into carbon nanofibers 沼气转化为纳米碳纤维的串联催化策略

IF 9.4

Chem Catalysis Pub Date : 2025-04-17 DOI: 10.1016/j.checat.2025.101363

Hefei Li, Feng Jiao

引用次数: 0

Stabilizing metal nanoparticle catalysts in their dynamic processes 稳定金属纳米颗粒催化剂的动态过程

IF 9.4

Chem Catalysis Pub Date : 2025-04-17 DOI: 10.1016/j.checat.2025.101330

Lujie Liu, Wentao Yuan, Siyu Yao, Ang Cao, Liang Wang

引用次数: 0

Iridium nanoparticles embedded in ceria set a new benchmark for PEM water electrolyzers 在铈中嵌入铱纳米颗粒为PEM水电解槽树立了新的标杆

IF 9.4

Chem Catalysis Pub Date : 2025-04-17 DOI: 10.1016/j.checat.2025.101355

David Hernández-Castillo, Kai S. Exner

引用次数: 0

How distorted nanotwins boost hydrogen evolution 扭曲的纳米孪晶如何促进氢的演化

IF 9.4

Chem Catalysis Pub Date : 2025-04-17 DOI: 10.1016/j.checat.2025.101362

Marie-Ingrid Richard, Clément Atlan

引用次数: 0

Interfacial structure engineering enhances photo-thermal CO2 hydrogenation over Ni-CeO2 nanocomposites 界面结构工程增强Ni-CeO2纳米复合材料的光热CO2加氢作用

IF 9.4

Chem Catalysis Pub Date : 2025-04-17 DOI: 10.1016/j.checat.2025.101361

Shikang Xiao, Lige Wang, Yunxiang Tang, Zhengyi Yang, Hao Wang, Chan Guo, Tingting Zhao, Yanyan Jiang, Xiaodong Wen, Fenglong Wang

{"title":"Interfacial structure engineering enhances photo-thermal CO2 hydrogenation over Ni-CeO2 nanocomposites","authors":"Shikang Xiao, Lige Wang, Yunxiang Tang, Zhengyi Yang, Hao Wang, Chan Guo, Tingting Zhao, Yanyan Jiang, Xiaodong Wen, Fenglong Wang","doi":"10.1016/j.checat.2025.101361","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101361","url":null,"abstract":"Metal-support interfaces play pivotal roles in governing the catalytic behaviors in heterogeneous catalysts, yet their optimized construction remains a formidable challenge. Here, we delve into the role of nickel-ceria interfaces in enhancing photo-thermal CO2 hydrogenation by designing a series of Ni/CeO2 composite catalysts with distinct interfacial features. The one with a well-defined nickel-ceria interface, achieved through lattice matching, demonstrates an exceptional CH4 production rate of 477.3 mmol gcat−1 h−1 (99.7% selectivity, 89.4% CO2 conversion) at 250°C under ambient pressure and light irradiation (200–1,100 nm, 2740 mW cm−2). This remarkable performance is credited to the distinctive metal-support interaction and efficient charge transfer at the interface. In contrast, catalysts lacking lattice-matched interfaces or featuring encapsulated nickel nanoparticles show inferior activity due to inhibited charge transfer and restricted access to active sites. These findings underscore the importance of interface engineering in optimizing photo-thermal catalysts for CO2 hydrogenation.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"28 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143842105","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

Spatially asymmetric catalyst design with electron-rich Cu sites to facilitate full-spectrum photo-Fenton-like catalysis 空间不对称催化剂设计，具有富电子的Cu位点，促进全谱光芬顿催化

IF 9.4

Chem Catalysis Pub Date : 2025-04-17 DOI: 10.1016/j.checat.2025.101358

Wei Zhang, Lan Wang, Fu Wang, Mingyang Xing, Chuanyi Wang, Jincai Zhao

{"title":"Spatially asymmetric catalyst design with electron-rich Cu sites to facilitate full-spectrum photo-Fenton-like catalysis","authors":"Wei Zhang, Lan Wang, Fu Wang, Mingyang Xing, Chuanyi Wang, Jincai Zhao","doi":"10.1016/j.checat.2025.101358","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101358","url":null,"abstract":"Heterogeneous photo-Fenton catalysis stands out as a promising advanced oxidation technology but is subject to slow reaction kinetics because the electron supply is insufficient to sustain the Fenton reaction. Here, we demonstrate an asymmetric-catalyst-based copper silicate nanotube (CSN) Janus design that simultaneously enables favorable full-spectrum solar absorption, H2O2 adsorption, and catalytic activity. The coordination asymmetry induces oxygen-vacancy-associated, electron-rich Cu(I) sites and an intrinsic electric field oriented from the Si-O to the Cu-O sublayer, synergistically driving the photoexcited electrons to compensate for the electron-donating capability of Cu sites, leading to remarkably enhanced H2O2 activation. The strong electron delocalization of Cu(I) sites reinforces the H2O2 adsorption on its adjacent bridging H sites. The energy barrier for H2O2 dissociation is vastly reduced (0.912 → 0.264 eV), boosting H2O2 utilization (54%, almost two times higher than that of conventional catalysts). The CSN-catalyzed photo-Fenton-like reaction attains long-lasting ·OH production, which affords exceptional performance for various types of organic pollutant elimination.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"58 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143842106","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