物理化学学报2026，Vol.42Issue(7)：211-227,17.DOI:10.1016/j.actphy.2026.100287
电子结构不对称碳介导的Pd电荷重分布促进乙醇氧化反应
Charge redistribution on Pd mediated by electronically asymmetric carbon for boosting ethanol oxidation
摘要
Abstract
Pd-based materials as the promising catalysts for ethanol oxidation reaction(EOR)are still intrinsically limited by the surface electronic-structure trade-off between ethanol adsorption and CH3CO intermediate desorption.Herein,the Pd supported on N/S co-doped carbon(Pd@SNC)catalyst is synthesized,in which the doped S and N atoms could transfer moderate amounts electron to Pd,leading to opportune electron structure of Pd.Moreover,the moderate negative shift of d-band center demonstrate that the opportune Pd electron structure can strengthen adsorption of ethanol/OH-and promote the desorption of intermediate(CH3CO*),which may facilitate the kinetics.As a result,Pd@SNC exhibiting the highest catalytic activity for EOR(945.49 mA mgPd-1),surpassing to that of Pd@NC and Pd@C.Due to the fact that the electronic structure of Pd is properly regulated by co-doped N and S atoms,as shown by the theoretical calculation results,Pd@SNC exhibits the lowest reaction energy barrier of the dehydrogenation during the process of EOR.关键词
Pd基催化剂/乙醇氧化/杂原子掺杂/金属-载体相互作用/电子结构Key words
Pd-based catalyst/Ethanol oxidation/Heteroatoms doping/Metal-support interaction/Electronic structure分类
化学化工引用本文复制引用
周鑫灿,吴广磊,王雪瑶,陈小康,兰笛,高宇庭,王晓霞,李道浩,张树超,张立杰..电子结构不对称碳介导的Pd电荷重分布促进乙醇氧化反应[J].物理化学学报,2026,42(7):211-227,17.基金项目
本工作得到了国家自然科学基金8257028和52377026)、泰山学者计划(tsqn202211124和tsqn202103057)、山东省自然科学基金(ZR2022QB023)以及山东省高等学校青创人才引育计划(海洋多糖纤维基能源材料研究与创新团队)的资助. （tsqn202211124和tsqn202103057）
