Elucidating the origin of catalytic activity of nitrogen-doped carbon coated nickel toward electrochemical reduction of CO2

Qingting Zeng; Guangxing Yang; Qiao Zhang; Zhiting Liu; Chengxiong Dang; Binhao Qin; Feng Peng

doi:10.1016/j.jcis.2023.06.198

Elucidating the origin of catalytic activity of nitrogen-doped carbon coated nickel toward electrochemical reduction of CO₂

J Colloid Interface Sci. 2023 Nov 15;650(Pt A):132-142. doi: 10.1016/j.jcis.2023.06.198. Epub 2023 Jun 29.

Authors

Qingting Zeng¹, Guangxing Yang¹, Qiao Zhang¹, Zhiting Liu¹, Chengxiong Dang¹, Binhao Qin², Feng Peng³

Affiliations

¹ School Chemistry and Chemical Engineering, Guangzhou University, Guangzhou 510006, China.
² China-Ukraine Institute of Welding, Guangdong Academy of Sciences, Guangdong Provincial Key Laboratory of Advanced Welding Technology, Guangzhou 510650, China. Electronic address: qinbinhao@yeah.net.
³ School Chemistry and Chemical Engineering, Guangzhou University, Guangzhou 510006, China. Electronic address: fpeng@gzhu.edu.cn.

PMID: 37399749
DOI: 10.1016/j.jcis.2023.06.198

Abstract

Converting CO₂ into valuable chemicals and fuels through clean and renewable energy electricity provides a way to achieve sustainable development for human societies. In this study, carbon coated nickel catalysts (Ni@NCT) were prepared by solvothermal and high-temperature pyrolysis methods. A series of Ni@NC-X catalysts were obtained by pickling with different kinds of acids for electrochemical CO₂ reduction reaction (ECRR). The results show that Ni@NC-N treated with nitric acid has the highest selectivity but lower activity, Ni@NC-S treated with sulfuric acid has the lowest selectivity, and Ni@NC-Cl treated with hydrochloric acid shows the best activity and good selectivity. At -1.16 V, Ni@NC-Cl has a considerable CO yield of 472.9 μmol h^-1 cm^-2, which is significantly superior to Ni@NC-N (327.5), Ni@NC-S (295.6) and Ni@NC (270.8). The controlled experiments show that there is a synergistic effect between Ni and N. The chlorine adsorbed on the surface can promote the performance of ECRR. The poisoning experiments indicate that the contribution of surface Ni atoms to the ECRR is very small, and the increase of activity is mainly due to the nitrogen doped carbon coated Ni particles. The relationship between activity and selectivity of ECRR on different acid-washed catalysts was correlated by theoretical calculations for the first time, which is also in good agreement with the experimental results.

Keywords: Acid treatment; Active sites; Carbon catalysis; Carbon-encapsulated nickel catalyst; Electrochemical CO(2) reduction; Nitrogen-doped carbon.