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Electrochemical Oxidation of CO on Cu Single Crystals under Alkaline Conditions
ACS Energy Letters ( IF 19.3 ) Pub Date : 2020-10-15 , DOI: 10.1021/acsenergylett.0c01751 Aarti Tiwari 1 , Hendrik H. Heenen 1 , Anton Simon Bjørnlund 1 , Degenhart Hochfilzer 1 , Karen Chan 1 , Sebastian Horch 1, 2
ACS Energy Letters ( IF 19.3 ) Pub Date : 2020-10-15 , DOI: 10.1021/acsenergylett.0c01751 Aarti Tiwari 1 , Hendrik H. Heenen 1 , Anton Simon Bjørnlund 1 , Degenhart Hochfilzer 1 , Karen Chan 1 , Sebastian Horch 1, 2
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We perform a joint experimental–theoretical study of the electrochemical oxidation of CO on copper (Cu) under alkaline conditions. Using cyclic voltammetry on Cu single-crystal surfaces, we demonstrate that both Cu terraces and steps show CO oxidation activity at potentials just slightly positive (0.03–0.14 V) of the thermodynamic equilibrium potential. The overpotentials are 0.23–0.12 V lower than that of gold (≈0.26 V), which until now has been considered to be the most active catalyst for this process. Our theoretical calculations suggest that Cu’s activity arises from the advantageous combination of simultaneous *CO and *OH adsorption under CO oxidation potentials and surmountable *CO–*OH coupling barriers. Experimentally observed onset potentials are in agreement with the computed onsets of *OH adsorption. We furthermore show that the onsets of *OH adsorption on steps are more affected by *CO–*OH interactions than on terraces due to a stronger competitive adsorption. Overall, Cu(100) shows the lowest overpotential (0.03 V) of the facets considered.
中文翻译：
碱性条件下CO在Cu单晶上的电化学氧化
我们进行了碱性条件下CO在铜（Cu）上的电化学氧化的联合实验理论研究。在铜单晶表面上使用循环伏安法，我们证明了铜阶跃和阶梯都显示出在热力学平衡电势略微为正（0.03-0.14 V）的电势下的CO氧化活性。过电势比金（≈0.26V）低0.23–0.12 V，迄今为止，金被认为是该过程中活性最高的催化剂。我们的理论计算表明，铜的活性来自同时* CO和* OH在CO氧化电位下的吸附和可克服的* CO- * OH耦合势垒的有利结合。实验观察到的起始电位与* OH吸附的计算起始相符。我们进一步表明，由于强竞争吸附，台阶上* OH吸附的开始受* CO- * OH相互作用的影响要比台阶上更多。总体而言，Cu（100）在所考虑的方面显示出最低的过电势（0.03 V）。
更新日期：2020-11-13
中文翻译：
碱性条件下CO在Cu单晶上的电化学氧化
我们进行了碱性条件下CO在铜（Cu）上的电化学氧化的联合实验理论研究。在铜单晶表面上使用循环伏安法，我们证明了铜阶跃和阶梯都显示出在热力学平衡电势略微为正（0.03-0.14 V）的电势下的CO氧化活性。过电势比金（≈0.26V）低0.23–0.12 V，迄今为止，金被认为是该过程中活性最高的催化剂。我们的理论计算表明，铜的活性来自同时* CO和* OH在CO氧化电位下的吸附和可克服的* CO- * OH耦合势垒的有利结合。实验观察到的起始电位与* OH吸附的计算起始相符。我们进一步表明，由于强竞争吸附，台阶上* OH吸附的开始受* CO- * OH相互作用的影响要比台阶上更多。总体而言，Cu（100）在所考虑的方面显示出最低的过电势（0.03 V）。
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