Kun Ma1, Songliang Liu1*, Huaifang Teng1, Weixin Miao1, Xiaotong Zhou1, Xuejing Cui1, Xin Zhou2,3* and Luhua Jiang1*
1Electrocatalysis & Nanomaterial Laboratory, College of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, China.
2Interdisciplinary Research Center for Biology and Chemistry, Liaoning Normal University, Dalian, Liaoning, 116029, P. R. China.
3College of Environment and Chemical Engineering, Dalian University, Dalian 116622, P. R. China.
Corresponding author
*E-mail: liusongliang@qust.edu.cn, zhouxin@dlu.edu.cn, luhuajiang@qust.edu.cn
ABSTRACT:
Electro-oxidation of ethanol, as the anodic reaction of direct ethanol fuel cells, is crucial for discharging performance. However, the kinetics of C-C bond cleavage in ethanol is very sluggish at low temperatures, due to the lack of efficient electrocatalysts. In this work, a unique tensile-strained defect-rich PdCo bimetallene nanoribbons (PdCo BNRs) is constructed, which exhibits a graphene-like nanoribbon structure with ultrathin thickness and abundant structural defects. As expected, the optimized PdCo BNRs exhibits an excellent ethanol oxidation activity (1.47 A mg−1) as well as a super C-C bond cleavage capability and high selectivity for C1 products (49.2%), compared with Pd metallene nanoribbons and commercial Pd black. Density-functional theory calculations combined with in-situ electrochemical Fourier transform infrared spectroscopy shows that the highly oxygenophilic Co and the unique tensile strain effect effectively upshift the d-band center of Pd to promote the adsorption of *OH, and most of all, significantly lower the activation energy barriers for C-C bond cleavage and accelerate the oxidation of CO*. This work not only provides an effective strategy for optimization of electron configuration of metallene nanoribbons, but also provides a guidance for the rational design of efficient catalysts for C-C bond cleavage in ethanol oxidation reaction.
KEYWORDS: PdCo bimetallene nanoribbons, defect, tensile-strain, electrocatalysts, ethanol oxidation reaction
