Electrochemically-induced highly reactive PdO^(*) interface on modulated mesoporous MOF-derived Co_(3)O_(4) support for selective ethanol electro-oxidation  

作　　者：Yuling Chen Yali Wen Qun Zhou Lina Shen Fanghui Du Pai Peng Yu Chen Junwei Zheng 

机构地区：[1]College of Chemistry,Chemical Engineering and Materials Science&Collaborative Innovation Center of Suzhou Nano Science and Technology,Soochow University,Suzhou 215123,Jiangsu,China [2]School of Materials Science and Engineering,Yancheng Institute of Technology,Yancheng 224051,Jiangsu,China [3]Shandong Provincial Key Laboratory of Chemical Energy Storage and Novel Cell Technology and School of Chemistry and Chemical Engineering,Liaocheng University,Liaocheng 252000,Shandong,China

出　　处：《Journal of Energy Chemistry》2023年第11期609-619,I0013,共12页能源化学（英文版）

基　　金：supported by the National Natural Science Foundation of China(21336005);the Ministry of Science and Technology of China(2014EG111224);the National Key R&D Program of China(2021YFB4001200);the Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX22_3185)。

摘　　要：Herein,Pd nanoparticles loaded Co_(3)O_(4)catalysts(Pd@Co_(3)O_(4))are constructed from zeolitic imidazolate framework-67(ZIF-67)for the ethanol oxidation reaction(EOR).It is demonstrated for the first time that the electrochemical conversion of Co_(3)O_(4)support would result in the charge distribution alignment at the Pd/Co_(3)O_(4)interface and induce the formation of highly reactive Pd-O species(PdO^(*)),which can further catalyze the consequent reactions of the intermediates of the ethanol oxidation.The catalyst,Pd@Co_(3)O_(4)-450,obtained under the optimized conditions exhibits excellent EOR performance with a high mass activity of 590 mA mg-1,prominent operational stability,and extraordinary capability for the electro-oxidation of acetaldehyde intermediates.Importantly,the detailed mechanism investigation reveals that Pd@Co_(3)O_(4)-450 could be benefit to the C-C bond cleavage to promote the desirable C1 pathway for the ethanol oxidation reaction.The present strategy based on the metal-support interaction of the catalyst might provide valuable inspiration for the design of high-performing catalysts for the ethanol oxidation reaction.

关 键 词：ZIF-67 derived Co_(3)0_(4) Reactive PdO^(*)species Mesoporous hollow structure Ethanol electro-oxidation Acetaldehyde electro-oxidation 

分 类 号：O643.36[理学—物理化学]