Chem Catalysis最新文献_第2页

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

Facile access to allylgermanes via nickela-electrocatalyzed germylative allylation 通过镍电催化的萌发性烯丙基化，易于获得烯丙基日耳曼

IF 9.4

Chem Catalysis Pub Date : 2025-04-17 DOI: 10.1016/j.checat.2025.101360

Xiaolin Ren, Yuan Huang

引用次数: 0

Regulating electronic density and interfacial electric field of high-entropy metallenes to enhance oxygen reduction reaction activity 调节高熵金属烯的电子密度和界面电场，提高氧还原反应活性

IF 9.4

Chem Catalysis Pub Date : 2025-04-15 DOI: 10.1016/j.checat.2025.101357

Wenning Liu, Li An, Pengfei Li, Yajie Fu, Xu Zhang, Dan Qu, Yichang Liu, Pu Hu, Xiayan Wang, Ning Jiang, Zaicheng Sun

{"title":"Regulating electronic density and interfacial electric field of high-entropy metallenes to enhance oxygen reduction reaction activity","authors":"Wenning Liu, Li An, Pengfei Li, Yajie Fu, Xu Zhang, Dan Qu, Yichang Liu, Pu Hu, Xiayan Wang, Ning Jiang, Zaicheng Sun","doi":"10.1016/j.checat.2025.101357","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101357","url":null,"abstract":"High-entropy metallenes (HEMs), combining high-entropy alloys and ultrathin nanosheets, exhibit lattice strain, geometric effects, and electronic modulation, enhancing oxygen reduction reaction (ORR) activity. We propose a strategy to manipulate the interfacial electric field and electronic density of states in HEMs by adjusting atomic radius and electronegativity differences. Integrating smaller atomic radius elements (Fe/Co/Ni) with larger ones (Pt/Pd/Mo) increases nanosheet curvature, altering the local electric field. Low-electronegativity Fe/Co/Ni/Mo elements lower the d-band center of Pd, and Pt further decreases it, reducing oxygen intermediate adsorption energy. PtPdFeCoNiMo HEMs, with sub-nanometer thickness, high curvature, microstrain, and optimized electronic structure, achieve ORR mass activity of 1.40 A·mgPt−1 at 0.9 V (vs. reversible hydrogen electrode [RHE]) in 0.1 M KOH, 21 times higher than Pt/C. They retain excellent performance after 20,000 cycles, with reduced energy barriers for the rate-determining ORR step.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"5 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143832191","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

Promoting CO2 reduction in the presence of oxygen with polymer-based gas diffusion electrodes 聚合物基气体扩散电极在氧气存在下促进CO2的还原

IF 9.4

Chem Catalysis Pub Date : 2025-04-10 DOI: 10.1016/j.checat.2025.101353

Sam Van Daele, Lieven Hintjens, Daniel Choukroun, Nick Daems, Jonas Hereijgers, Tom Breugelmans

引用次数: 0

Paired electrochemical synthesis of glycolic acid and ammonia from polyester and nitrate sewage 从聚酯和硝酸盐污水中配对电化学合成乙醇酸和氨水

IF 9.4

Chem Catalysis Pub Date : 2025-04-07 DOI: 10.1016/j.checat.2025.101336

Yingxin Ma, Xuyun Guo, Wenfang Yuan, Peinuo Yang, Yu Zhang, Wenxuan Chen, Lejuan Cai, Valeria Nicolosi, Wenlong Wang, Yang Chai, Bocheng Qiu

{"title":"Paired electrochemical synthesis of glycolic acid and ammonia from polyester and nitrate sewage","authors":"Yingxin Ma, Xuyun Guo, Wenfang Yuan, Peinuo Yang, Yu Zhang, Wenxuan Chen, Lejuan Cai, Valeria Nicolosi, Wenlong Wang, Yang Chai, Bocheng Qiu","doi":"10.1016/j.checat.2025.101336","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101336","url":null,"abstract":"Electrochemical upcycling of nitrate (NO3−) wastewater to ammonia offers a sustainable route for reclaiming nitrogen resources from waste. However, its practical implementation still faces substantial obstacles, including high energy input and limited selectivity. Here, we report a paired electrochemical system that combines the anodic oxidation of polyethylene terephthalate (PET) hydrolysate, specifically its ethylene glycol (EG) monomer, to glycolic acid (GA) with the cathodic reduction of NO3− to ammonia. All of this is made possible by the discovery of a PdCu alloy anode and a CuCo alloy cathode. Built upon experimental demonstration and a theoretical understanding of the improved CO resistance on the PdCu alloy for EG oxidation, as well as the synergy between Cu and Co for NO3− reduction, our paired system enables the efficient co-production of GA and ammonia from PET hydrolysate and NO3−-containing wastewater. This conceptual design of paired electrochemistry provides an intriguing way to synthesize high-value chemicals from waste resources.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"21 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143790049","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

Oxygen-vacancy-mediated photocatalytic activity of antimony molybdenum oxide toward green ammonia synthesis 氧空位介导的氧化锑钼光催化活性在绿色氨合成中的应用

IF 9.4

Chem Catalysis Pub Date : 2025-04-04 DOI: 10.1016/j.checat.2025.101337

Botong Liu, Ling Huang, Terence Musho, Chih-Jung Chen, Chung-Li Dong, Chaoyun Tang, Alhassan Yasin, Yulei Wang, Hui Yang, Joeseph Bright, Peng Zheng, Ru-Shi Liu, Nianqiang Wu

{"title":"Oxygen-vacancy-mediated photocatalytic activity of antimony molybdenum oxide toward green ammonia synthesis","authors":"Botong Liu, Ling Huang, Terence Musho, Chih-Jung Chen, Chung-Li Dong, Chaoyun Tang, Alhassan Yasin, Yulei Wang, Hui Yang, Joeseph Bright, Peng Zheng, Ru-Shi Liu, Nianqiang Wu","doi":"10.1016/j.checat.2025.101337","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101337","url":null,"abstract":"Oxygen vacancies in metal oxide photocatalysts are essential to activate photocatalytic activity toward nitrogen fixation, although their roles and underlying mechanisms remain poorly understood. Unfortunately, oxygen vacancies are prone to disappear during photocatalysis processes. Herein, antimony molybdate (Sb2MoO6) is proposed as a photocatalyst for green ammonia synthesis, which achieves ammonia generation rate of 6.39 μM h−1⋅g−1. Oxygen vacancies modulate the MoO6 octahedra, not the tetrahedral, SbO4 bilayers in the triclinic structure of Sb2MoO6 and result in partial reduction of Mo6+ to Mo5+. Instead of oxygen vacancies themselves, Mo5+ serves as active sites, favoring surface adoption of N2 and formation of reaction intermediates. Oxygen vacancies are predominantly refilled over extended photocatalysis, leading to conversion of Mo5+ back to Mo6+ and consequent photocatalyst deactivation. Therefore, cobalt dopant is introduced to stabilize the oxygen vacancies effectively. The scientific insights obtained will guide the development of stable photocatalysts for green ammonia synthesis.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"13 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143776201","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

Cooperative effects associated with high electrolyte concentrations in driving the conversion of CO2 to C2H4 on copper 高浓度电解质在推动铜上 CO2 向 C2H4 转化过程中的协同效应

IF 9.4

Chem Catalysis Pub Date : 2025-04-04 DOI: 10.1016/j.checat.2025.101338

Shaoyang Lin, Yuval Fishler, Soonho Kwon, Annette E. Böhme, Weixuan Nie, Matthias H. Richter, Moon Young Yang, Jesse E. Matthews, Zachery W.B. Iton, Brian C. Lee, Thomas F. Jaramillo, Harry A. Atwater, William A. Goddard, Wilson A. Smith, Kimberly A. See

{"title":"Cooperative effects associated with high electrolyte concentrations in driving the conversion of CO2 to C2H4 on copper","authors":"Shaoyang Lin, Yuval Fishler, Soonho Kwon, Annette E. Böhme, Weixuan Nie, Matthias H. Richter, Moon Young Yang, Jesse E. Matthews, Zachery W.B. Iton, Brian C. Lee, Thomas F. Jaramillo, Harry A. Atwater, William A. Goddard, Wilson A. Smith, Kimberly A. See","doi":"10.1016/j.checat.2025.101338","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101338","url":null,"abstract":"Compared to a conventional electrolyte concentration of 1 M HCOOK, the use of a highly concentrated 7.1 M HCOOK electrolyte increases the Faradaic efficiency (FE) ratio of C2H4/CO from 2.2 ± 0.3 to 18.3 ± 4.8 at −1.08 V vs. reversible hydrogen electrode (RHE) on a Cu gas-diffusion electrode. Based on electrochemical analysis and ab initio molecular dynamics (AIMD) simulation, the identity and concentration of the cation and anion play more important roles in controlling the CO2R reaction pathway than the bulk CO2 solubility and the bulk pH of electrolytes. In situ attenuated reflectance surface enhanced infrared absorption spectroscopy (ATR-SEIRAS) suggests that, unlike 1 M HCOOK, the ∗CO-bridge-binding mode on Cu is dominant in 7.1 M HCOOK electrolyte, which potentially results in less CO release and higher yield of C2H4. This study demonstrates that although we can tailor the electrolyte composition to shift product selectivity, the factors that control the product selectivity are numerous and cannot be distilled down into one correlated property-reactivity relationship.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"1 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143776200","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

Suppressing lattice oxygen oxidation in ruthenium oxide via equivalent substitution for sustainable oxygen evolution reaction in PEMWEs 通过等效取代持续析氧反应抑制氧化钌中的晶格氧氧化

IF 9.4

Chem Catalysis Pub Date : 2025-04-03 DOI: 10.1016/j.checat.2025.101335

Xiaojie Chen, Rongpeng Ma, Wenqi Jia, Xuejie Cao, Jinyang Zhang, Fangyi Cheng, Lifang Jiao

{"title":"Suppressing lattice oxygen oxidation in ruthenium oxide via equivalent substitution for sustainable oxygen evolution reaction in PEMWEs","authors":"Xiaojie Chen, Rongpeng Ma, Wenqi Jia, Xuejie Cao, Jinyang Zhang, Fangyi Cheng, Lifang Jiao","doi":"10.1016/j.checat.2025.101335","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101335","url":null,"abstract":"Developing cost-effective Ru-based electrocatalysts for the acidic oxygen evolution reaction (OER) is crucial for proton-exchange membrane water electrolyzers (PEMWEs). However, the prominent lattice-oxygen-mediated mechanism (LOM) at high oxidative potential leads to crystal destruction and poor operational stability for RuO2. Here, we report that introducing equivalent Ti4+ into RuO2 can significantly suppress the oxidation of lattice oxygen. Spectroscopic and theoretical results demonstrate that Ti4+ incorporation not only decreases the LOM ratio by weakening Ru–O bond covalency but also suppresses the dynamic activation of lattice oxygen at high oxidative bias by inhibiting Ru–O bond contraction. Potential-resolved differential electrochemical mass spectrometry (DEMS) verified the decreased LOM ratio (from 53.45% to 5% at 1.8 V) after Ti4+ incorporation. The equivalent-Ti4+-substituted RuO2 not only exhibits an extended operation time of over 500 h at 100 mA cm−2 but also withstands fluctuating voltage input (1.5–1.8 V) for 120 h in PEMWEs.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"73 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766700","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

SubTuner leverages physics-based modeling to complement AI in enzyme engineering toward non-native substrates SubTuner利用基于物理的建模来补充AI在酶工程对非天然底物

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 钯催化伯烷基胺的α-芳基化反应

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