Spectroscopic Observation of Reversible Surface Reconstruction of Copper Electrodes under CO2 Reduction
Spectroscopic Observation of Reversible Surface Reconstruction of Copper Electrodes under CO2 Reduction
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DOI：
10.1021/acs.jpcc.7b03910
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发表时间：
2017-06-08
影响因子：
3.7
通讯作者：
Waegele, Matthias M.
中科院分区：
文献类型：
--
作者：
Gunathunge, Charuni M.;Li, Xiang;Waegele, Matthias M.
铜催化CO2电化学还原的能力很大程度上取决于其纳米级表面形貌。虽然以前的研究发现了电解后铜纳米颗粒和薄膜电极不可逆变化的证据，但我们在这里首次观察到吸附CO中间体诱导的电催化铜表面的可逆重建。利用衰减全内反射红外光谱和表面增强拉曼光谱，通过CO与下配位铜原子结合的新的C等效O吸收带的出现和表面增强拉曼效应的强烈增强，揭示了电极上纳米级金属团簇的可逆形成。我们的研究表明，催化铜表面的形态不是静态的，而是随着反应条件的变化而动态适应的。
The ability of copper to catalyze the electrochemical reduction of CO2 has been shown to greatly depend on its nanoscale surface morphology. While previous studies found evidence of irreversible changes of copper nanoparticle and thin film electrodes following electrolysis, we present here the first observation of the reversible reconstruction of electrocatalytic copper surfaces induced by the adsorbed CO intermediate. Using attenuated total internal reflection infrared and surface-enhanced Raman spectroscopies, the reversible formation of nanoscale metal clusters on the electrode is revealed by the appearance of a new C equivalent to O absorption band characteristic of CO bound to under coordinated copper atoms and by the strong enhancement of the surface-enhanced Raman effect. Our study shows that the morphology of the catalytic copper surface is not static but dynamically adapts with changing reaction conditions.