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Grain-Boundary-Rich Copper for Efficient Solar-Driven Electrochemical CO2 Reduction to Ethylene and Ethanol
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2020-03-27 , DOI: 10.1021/jacs.0c00971 Zhiqiang Chen 1 , Tuo Wang 1 , Bin Liu 1 , Dongfang Cheng 1 , Congling Hu 1 , Gong Zhang 1 , Wenjin Zhu 1 , Huaiyuan Wang 1 , Zhi-Jian Zhao 1 , Jinlong Gong 1
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2020-03-27 , DOI: 10.1021/jacs.0c00971 Zhiqiang Chen 1 , Tuo Wang 1 , Bin Liu 1 , Dongfang Cheng 1 , Congling Hu 1 , Gong Zhang 1 , Wenjin Zhu 1 , Huaiyuan Wang 1 , Zhi-Jian Zhao 1 , Jinlong Gong 1
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The grain boundary in copper-based electrocatalysts has been demon-strated to improve the selectivity of solar-driven electrochemical CO2 reduction towards multi-carbon products. However, the approach to form grain boundaries in copper is still limited. This paper describes a controllable grain growth of copper electrodeposition via poly (vinylpyr-rolidone) used as an additive. A grain-boundary-rich metallic copper could be obtained to convert CO2 into ethylene and ethanol with a high selectivity of 70% over a wide potential range. In-situ attenuated total reflection surface-enhanced infrared absorption spectroscopy unveils that the existence of grain boundaries enhances the adsorption of the key intermediate (*CO) on the copper surface to boost the further CO2 reduction. When coupling with a commercially available Si solar cell, the device achieves a remarkable solar-to-C2-products conversion efficiency of 3.88% at a large current density of 52 mA∙cm-2. This low-cost and efficient device is promising for large-scale application of solar-driven CO2 reduction.
中文翻译：
用于高效太阳能驱动电化学 CO2 还原为乙烯和乙醇的富晶界铜
铜基电催化剂中的晶界已被证明可以提高太阳能驱动的电化学 CO2 还原对多碳产品的选择性。然而，在铜中形成晶界的方法仍然有限。本文描述了通过用作添加剂的聚（乙烯基吡咯烷酮）进行铜电沉积的可控晶粒生长。可以获得富含晶界的金属铜，以在很宽的电位范围内以 70% 的高选择性将 CO2 转化为乙烯和乙醇。原位衰减全反射表面增强红外吸收光谱揭示了晶界的存在增强了关键中间体 (*CO) 在铜表面上的吸附，从而促进了进一步的 CO2 还原。当与市售的硅太阳能电池耦合时，该器件在 52 mA∙cm-2 的大电流密度下实现了 3.88% 的太阳能到 C2 产品的卓越转换效率。这种低成本、高效的装置有望大规模应用太阳能驱动的 CO2 减排。
更新日期：2020-03-27
中文翻译：
用于高效太阳能驱动电化学 CO2 还原为乙烯和乙醇的富晶界铜
铜基电催化剂中的晶界已被证明可以提高太阳能驱动的电化学 CO2 还原对多碳产品的选择性。然而，在铜中形成晶界的方法仍然有限。本文描述了通过用作添加剂的聚（乙烯基吡咯烷酮）进行铜电沉积的可控晶粒生长。可以获得富含晶界的金属铜，以在很宽的电位范围内以 70% 的高选择性将 CO2 转化为乙烯和乙醇。原位衰减全反射表面增强红外吸收光谱揭示了晶界的存在增强了关键中间体 (*CO) 在铜表面上的吸附，从而促进了进一步的 CO2 还原。当与市售的硅太阳能电池耦合时，该器件在 52 mA∙cm-2 的大电流密度下实现了 3.88% 的太阳能到 C2 产品的卓越转换效率。这种低成本、高效的装置有望大规模应用太阳能驱动的 CO2 减排。
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