Chen Chunjun, Yan Xupeng, Wu Ruizhi, Wu Yahui, Zhu Qinggong, Hou Minqiang, Zhang Zhaofu, Fan Honglei, Ma Jun, Huang Yuying, Ma Jingyuan, Sun Xiaofu, Lin Longfei, Liu Shoujie, Han Buxing
Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences Beijing 100190 P. R. China
University of Chinese Academy of Sciences Beijing 100049 China.
Chem Sci. 2021 Aug 10;12(35):11914-11920. doi: 10.1039/d1sc02328d. eCollection 2021 Sep 15.
Powered by a renewable electricity source, electrochemical CO reduction reaction is a promising solution to facilitate the carbon balance. However, it is still a challenge to achieve a desired product with commercial current density and high efficiency. Herein we designed quasi-square-shaped cadmium hydroxide nanocatalysts for CO electroreduction to CO. It was discovered that the catalyst is very active and selective for the reaction. The current density could be as high as 200 mA cm with a nearly 100% selectivity in a commonly used H-type cell using the ionic liquid-based electrolyte. In addition, the faradaic efficiency of CO could reach 90% at a very low overpotential of 100 mV. Density functional theory studies and control experiments reveal that the outstanding performance of the catalyst was attributed to its unique structure. It not only provides low Cd-O coordination, but also exposes high activity (002) facet, which requires lower energy for the formation of CO. Besides, the high concentration of CO can be achieved from the low concentration CO an adsorption-electrolysis device.
由可再生电源驱动，电化学CO还原反应是促进碳平衡的一种有前景的解决方案。然而，以商业电流密度和高效率实现所需产物仍然是一个挑战。在此，我们设计了用于CO电还原为CO的准方形氢氧化镉纳米催化剂。发现该催化剂对该反应具有很高的活性和选择性。在使用基于离子液体的电解质的常用H型电池中，电流密度可高达200 mA cm，选择性接近100%。此外，在仅100 mV的非常低的过电位下，CO的法拉第效率可达到90%。密度泛函理论研究和对照实验表明，该催化剂的优异性能归因于其独特的结构。它不仅提供了低的Cd-O配位，还暴露了高活性的(002)晶面，形成CO所需的能量更低。此外，通过低浓度CO吸附-电解装置可以实现高浓度的CO。
