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 e...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.展开更多
基金supported by the National Natural Science Foundation of China(21336005)the Ministry of Science and Technology of China(2014EG111224)+1 种基金the National Key R&D Program of China(2021YFB4001200)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX22_3185)。
文摘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.
