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作者机构:School of Materials Science and EngineeringCentral South UniversityChangsha 410083HunanChina State Key Laboratory of Advanced Technology for Materials Synthesis and ProcessingWuhan University of TechnologyWuhan 430070HubeiChina School of Physics and Electronic EngineeringJiangsu UniversityZhenjiang 212013JiangsuChina
出 版 物:《Chinese Journal of Catalysis》 (催化学报(英文))
年 卷 期:2021年第42卷第10期
页 面:1798-1807页
核心收录:
学科分类:081702[工学-化学工艺] 081705[工学-工业催化] 07[理学] 070205[理学-凝聚态物理] 08[工学] 0817[工学-化学工程与技术] 080501[工学-材料物理与化学] 080502[工学-材料学] 0805[工学-材料科学与工程(可授工学、理学学位)] 0702[理学-物理学]
基 金:国家自然科学基金(51572301) 国家重点研发项目(2017YFB0306000) 湖南省自然科学基金(2016JJ3153) 中南大学创新驱动项目(502221802) 中南大学双一流资助项目
主 题:Tungsten carbide Doping Surficial engineering Hydrogen evolution reaction Electrocatalyst
摘 要:Controllably mounting foreign atoms on the surfaces of earth-abundant electrocatalysts strongly improve their surface electronic properties for optimizing the catalytic performance of surficial sites to an unusual level,and provides a good platform to gain deep insights into catalytic *** present work describes,employing ultrafine W2C nanoislands(average size:2.3 nm)monodispersed on the N,P dual-doped carbon frameworks as a model system,how to regulate the atomic phosphorous-mounting effect on the surfaces of W_(2)C to derive an active and stable P-mounting W_(2)C(WCP)catalyst for both acidic and alkaline hydrogen evolution reaction(HER).Since in situ phosphorus substitution into carbon sites of preformed W_(2)C nanoislands gradually proceeds from surfaces to solids,so that using a proper amount of phosphorus sources can readily control the surface mounting level to avoid the mass P-doping into the *** this way,the activity per active site of WCP catalyst with robust stability can be optimized to 0.07 and 0.56 H_(2 )s^(-1) at-200 mV overpotential in acid and base,respectively,which reach up to the several-fold of pure-phase W_(2)C(0.01 and 0.05 H_(2) s^(-1)).Theoretical investigations suggest that compared with solid P doping,the P mounting on W_(2)C surface can more remarkably enhance its metallicity and decrease the hydrogen release *** finding disclosed a key correlation between surface foreign atom-mounting and catalytic activity,and suggested a logical extension to other earth-abundant catalysts for various catalytic reactions.