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Effects of Surface Roughness on the Electrochemical Reduction of CO2 over Cu
ACS Energy Letters ( IF 19.3 ) Pub Date : 2020-03-19 , DOI: 10.1021/acsenergylett.0c00482
Kun Jiang 1, 2, 3 , Yufeng Huang 4 , Guosong Zeng 5 , Francesca M. Toma 2, 5 , William A. Goddard 4 , Alexis T. Bell 2, 3, 5
Affiliation  

We have investigated the role of surface roughening on the CO2 reduction reaction (CO2RR) over Cu. The activity and product selectivity of Cu surfaces roughened by plasma pretreatment in Ar, O2, or N2 were compared with that of electrochemically polished Cu samples. Differences in total and product current densities, the ratio of current densities for HER (the hydrogen evolution reaction) to CO2RR, and the ratio of current densities for C2+ to C1 products depend on the electrochemically active surface and are nearly independent of plasma composition. Theoretical analysis of an electropolished and roughened Cu surface reveals a higher fraction of undercoordinated Cu sites on the roughened surface, sites that bind CO preferentially. Roughened surfaces also contain square sites similar to those on a Cu(100) surface but with neighboring step sites, which adsorb OC–COH, a precursor to C2+ products. These findings explain the increases in the formation of oxygenates and hydrocarbons relative to CO and the ratio of oxygenates to hydrocarbons observed with increasing surface roughness.

中文翻译:

表面粗糙度对铜上CO 2电化学还原的影响

我们已经研究了表面粗糙对Cu上CO 2还原反应(CO 2 RR)的作用。将通过等离子预处理在Ar,O 2或N 2中粗糙化的Cu表面的活性和产物选择性与电化学抛光的Cu样品的活性和产物选择性进行了比较。总电流密度和产物电流密度的差异,HER(析氢反应)的电流密度与CO 2 RR的比率以及C 2+到C 1的电流密度的比率产品取决于电化学活性表面,几乎与血浆成分无关。对经过电抛光和粗糙化的Cu表面的理论分析表明,在粗糙化的表面上有较高比例的配位不足的Cu位置,这些位置优先结合CO。粗糙的表面还包含类似于Cu(100)表面的正方形位置,但相邻的台阶位置会吸附OC-COH(C 2+产品的前体)。这些发现解释了随着表面粗糙度的增加,相对于CO,含氧化合物和碳氢化合物的形成增加,以及含氧化合物与碳氢化合物的比率增加。
更新日期:2020-04-23
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