镍单原子催化剂的制备及其电催化CO<sub>2</sub>还原研究

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摘要电催化CO₂还原反应(Electrocatalytic CO₂ reduction reaction, CO₂RR)在解决全球变暖和能源危机方面有着巨大的应用潜力,但目前催化效率低、催化产物多样等问题限制了CO₂RR反应的商业化应用。采用一锅法、碳化法制备了一系列不同镍含量的镍单原子催化剂,利用XRD、XPS、ICP-OES、HRTEM、HAADF-STEM、XAS等方法对镍单原子催化剂的形貌结构、原子价态、金属含量等方面进行表征,并通过电催化还原产物的法拉第效率(Faraday efficiency, FE)和电流密度(Current density, J)来评价其电催化性能。此外,还研究了电解实验装置的改变对升电催化性能的提升。实验结果表明,随着Ni单原子催化剂的Ni金属负载量增加,产物CO的FE_CO和J_CO均增加。催化剂中Zn₁Ni₂-CN表现出了优异的CO₂RR催化性能,在H型电解池中,在-0.7 V vs. RHE电位下FE_CO达到89%,在-0.9 V vs. RHE下J_CO达到6.99 mA·cm^-2。在流动电解池中,大范围电位变化下(-0.4~-1.2 V vs. RHE) FE_CO均保持在99%以上,且在-1.2 V vs. RHE电位下产物电流密度J_CO达到174.5 mA·cm^-2。

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	朱超
	张浩杰
	田地
	屈治国
	邸宏宇
	郑楠

关键词：镍单原子电催化 CO₂RR CO

Abstract： Electrocatalytic CO₂ reduction reaction (CO₂RR) has great application potential in solving global warming and the energy crisis, but the current problems such as low catalytic efficiency and diverse catalytic products limit the commercial application of CO₂RR reaction. A series of nickel single-atom catalysts with different nickel contents were prepared by a one-pot carbonization method. The morphology, structure, atomic valence state, and metal content of nickel single-atom catalysts were characterized by XRD, XPS, ICP-OES, HRTEM, HAADF-STEM, XAS and other methods. The electrocatalytic performance was evaluated by the Faradaic efficiency(FE) and current density(J) of the electrocatalytic reduction products. The electrocatalytic performance was improved by changing the electrolysis experimental device. The experimental results indicated that both FE_CO and J_CO increased as the Ni metal loading of Ni single-atom catalysts increased. Zn₁Ni₂-CN in the catalyst exhibited excellent CO₂RR catalytic performance. In the H-type electrolytic cell, the FE_CO reached 89% at -0.7 V vs. RHE, and the J_CO reached 6.99 mA·cm^-2 at -0.9 V vs. RHE. From -0.4 to -1.2 V vs. RHE in the flow electrolytic cell, FE_CO remained above 99%, and J_CO reached 174.5 mA·cm^-2 at -1.2 V vs. RHE.

Keywords： Ni-based single-atom catalyst electrocatalysis CO₂RR carbon monoxide

Received 2023-02-21;

Fund:国网陕西省电力有限公司科技项目(5226KY22001J)。

Corresponding Authors: 屈治国,教授,E-mail:zgqu@xjtu.edu.cn。 Email: zgqu@xjtu.edu.cn

About author: 朱超(1988-),男,在职博后,现从事新能源消纳的研究。

引用本文:

朱超, 张浩杰, 田地, 屈治国, 邸宏宇, 郑楠.镍单原子催化剂的制备及其电催化CO₂还原研究[J]. 化学工业与工程, 2024,41(3): 11-17

ZHU Chao, ZHANG Haojie, TIAN Di, QU Zhiguo, DI Hongyu, ZHENG Nan.Preparation and electrocatalytic CO₂ reduction of Ni-based single-atom catalyst[J]. Chemcial Industry and Engineering, 2024,41(3): 11-17

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