Accelerating Ethanol Complete Electrooxidation via Introducing Ethylene as the Precursor for the C-C Bond Splitting

被引:26
作者
Chen, Teng [1 ,2 ]
Xu, Shen [3 ]
Zhao, Taotao [2 ]
Zhou, Xiaohang [1 ]
Hu, Jianqiang [1 ]
Xu, Xin [1 ]
Liang, Chenjia [2 ]
Liu, Min [4 ]
Ding, Weiping [2 ]
机构
[1] Air Force Logist Acad, Xuzhou 221000, Jiangsu, Peoples R China
[2] Nanjing Univ, Sch Chem & Chem Engn, Nanjing 210023, Jiangsu, Peoples R China
[3] Nanyang Inst Technol, Sch Biol & Chem Engn, Nanyang 473004, Peoples R China
[4] Cent South Univ, Sch Phys & Elect, State Key Lab Powder Met, Changsha 410083, Hunan, Peoples R China
基金
中国国家自然科学基金; 中国博士后科学基金;
关键词
3D Printing; Dehydration; Ethanol Electrooxidation; Functional Support; Pt Nanoflowers; ALKALINE MEDIA; OXIDATION; ELECTRODE; PT/C; FTIR;
D O I
10.1002/anie.202308057
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The crucial issue restricting the application of direct ethanol fuel cells (DEFCs) is the incomplete and sluggish electrooxidation of ethanol due to the chemically stable C-C bond thereof. Herein, a unique ethylene-mediated pathway with a 100 % C1-selectivity for ethanol oxidation reaction (EOR) is proposed for the first time based on a well-structured Pt/Al2O3@TiAl catalyst with cascade active sites. The electrochemical in situ Fourier transform infrared spectroscopy (FTIR) and differential electrochemical mass spectrometry (DEMS) analysis disclose that ethanol is primarily dehydrated on the surface of Al2O3@TiAl and the derived ethylene is further oxidized completely on nanostructured Pt. X-ray absorption and density functional theory (DFT) studies disclose the Al component doped in Pt nanocrystals can promote the EOR kinetics by lowering the reaction energy barriers and eliminating the poisonous species. Strikingly, Pt/Al2O3@TiAl exhibits a specific activity of 3.83 mA cm(Pt)(-2), 7.4 times higher than that of commercial Pt/C and superior long-term durability.
引用
收藏
页数:6
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