Effects of Surface Roughness on the Electrochemical Reduction of CO2 over Cu,ACS Energy Letters

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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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