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内置电场在宽电位窗口下促进CO在C产物上的界面吸附和活化。

Built-in Electric Field Promotes Interfacial Adsorption and Activation of CO for C Products over a Wide Potential Window.

作者信息

Zhao Xin, Feng Qingguo, Liu Mengjie, Wang Yuchao, Liu Wei, Deng Danni, Jiang Jiabi, Zheng Xinran, Zhan Longsheng, Wang Jinxian, Zheng Huanran, Bai Yu, Chen Yingbi, Xiong Xiang, Lei Yongpeng

机构信息

State Key Laboratory of Powder Metallurgy, Central South University, Changsha 410083, People's Republic of China.

Key Laboratory of Advanced Technologies of Materials, Ministry of Education, Southwest Jiaotong University, Chengdu 610097, People's Republic of China.

出版信息

ACS Nano. 2024 Apr 2;18(13):9678-9687. doi: 10.1021/acsnano.4c01190. Epub 2024 Mar 24.

Abstract

The unsatisfactory adsorption and activation of CO suppress electrochemical reduction over a wide potential window. Herein, the built-in electric field (BIEF) at the CeO/InO n-n heterostructure realizes the C (CO and HCOO) selectivity over 90.0% in a broad range of potentials from -0.7 to -1.1 V with a maximum value of 98.7 ± 0.3% at -0.8 V. In addition, the C current density (-1.1 V) of the CeO/InO heterostructure with a BIEF is about 2.0- and 3.2-fold that of InO and a physically mixed sample, respectively. The experimental and theoretical calculation results indicate that the introduction of CeO triggered the charge redistribution and formed the BIEF at the interfaces, which enhanced the interfacial adsorption and activation of CO at low overpotentials. Furthermore, the promoting effect was also extended to CeO/InS. This work gives a deep understanding of BIEF engineering for highly efficient CO electroreduction over a wide potential window.

摘要

CO的吸附和活化效果不理想,这在很宽的电位窗口内抑制了电化学还原反应。在此,CeO/InO n-n异质结构中的内建电场(BIEF)在-0.7至-1.1 V的宽电位范围内实现了90.0%以上的C(CO和HCOO)选择性,在-0.8 V时最大值为98.7±0.3%。此外,具有BIEF的CeO/InO异质结构在-1.1 V时的C电流密度分别约为InO和物理混合样品的2.0倍和3.2倍。实验和理论计算结果表明,CeO的引入引发了电荷重新分布,并在界面处形成了BIEF,这增强了低过电位下CO的界面吸附和活化。此外,促进作用也扩展到了CeO/InS。这项工作为在宽电位窗口内高效CO电还原的BIEF工程提供了深入理解。

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