Single-Ni-atoms on nitrogenated humic acid based porous carbon for CO<sub>2</sub> electroreduction

doi:10.1007/s11705-024-2411-7

Front. Chem. Sci. Eng.

2024, Vol. 18

Issue (5) : 52 https://doi.org/10.1007/s11705-024-2411-7

Single-Ni-atoms on nitrogenated humic acid based porous carbon for CO₂ electroreduction

Delei Yu, Ying Chen, Yao Chen, Xiangchun Liu(

), Xianwen Wei(

), Ping Cui

Anhui Key Laboratory of Coal Clean Conversion & Utilization, School of Chemistry and Chemical Engineering, Anhui University of Technology, Ma’anshan 243002, China

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Abstract

We proposed a facile synthesis of single-Ni-atom catalysts on low-cost porous carbon using a calcination method at the temperatures of 850–1000 °C, which were used for CO₂ electrochemical reduction to CO. The porous carbon was prepared by carbonizing cheap and abundant humic acid. The structural characterizations of the as-synthesized catalysts and their electrocatalytic performances were analyzed. The results showed that the single-Ni-atom catalyst activated at 950 °C showed an optimum catalytic performance, and it reached a CO Faradaic efficiency of 91.9% with a CO partial current density of 6.9 mA·cm⁻² at −0.9 V vs. reversible hydrogen electrode (RHE). Additionally, the CO Faradaic efficiency and current density of the optimum catalyst changed slightly after 8 h of continuous operation, suggesting that it possessed an excellent stability. The structure-activity relations indicate that the variation in the CO₂ electrochemical reduction performance for the as-synthesized catalysts is ascribed to the combined effects of the increase in the content of pyrrolic N, the evaporation of Ni and N, the decrease in pore volume, and the change in graphitization degree.

Keywords CO₂ electroreduction single-Ni-atom catalysts humic acid based porous carbon

Corresponding Author(s): Xiangchun Liu,Xianwen Wei

Just Accepted Date: 12 January 2024 Issue Date: 12 April 2024

Cite this article:

Delei Yu,Ying Chen,Yao Chen, et al. Single-Ni-atoms on nitrogenated humic acid based porous carbon for CO₂ electroreduction[J]. Front. Chem. Sci. Eng., 2024, 18(5): 52.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-024-2411-7
https://academic.hep.com.cn/fcse/EN/Y2024/V18/I5/52

Fig.1 (a) FEs_CO on the as-prepared catalysts in the CO₂-saturated 0.1 mol·L^?1 KHCO₃ at different potentials; (b) FEs_CO and total current densities on Ni-N-HAPC-950 at different potentials; (c) CO partial current density (j_CO) values of the as-prepared catalysts; (d) FEs_CO and current densities on N-HAPC-950 and Ni-N-HAPC-950 at ?0.9 V_RHE; (e) linear sweep voltammetry curves of Ni-N-HAPC-950 collected in the CO₂- and Ar-saturated 0.1 mol·L^?1 KHCO₃ solutions.

Fig.2 (a) C_dl, (b) Tafel plots, and (c) electrochemical impedance spectra for HA, HAPC, and Ni-N-HAPC; (d) current-time response of Ni-N-HAPC-950 for CO₂ER at ?0.9 V_RHE.

Fig.3 SEM images of (a) HA, (b) HAPC, and (c–f) Ni-N-HAPC.

Fig.4 (a) SEM image of Ni-N-HAPC-950. (b) C, (c) N, (d) Ni, and (e) O elemental mappings.

Fig.5 (a) TEM and (b) HRTEM images for Ni-N-HAPC-950.

Fig.6 High resolution XPS spectra of N 1s for (a) HA, (b) HAPC, and (c–f) Ni-N-HAPC.

Fig.7 Relative contents of pyridinic, pyrrolic, graphitic, and oxidized N in all catalysts extracted from XPS.

Fig.8 Ni 2p XPS spectra of all catalysts.

Fig.9 XRD patterns of all catalysts.

Fig.10 Schematic of Ni-N-HAPC catalysts preparation and their CO₂ER mechanism.

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