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Research Article | Open Access

Tailoring the proximity of iron and manganese atomic sites for efficient CO2 electroreduction reaction

Xiaohui Sun1 (), Bangyan Zhang1, Qing Lu4, Jingjing Jiang5, Chenliang Ye2 (), Guoqing Cui1, Zechao Zhuang2, Jun Zhang4, Johannes H. Bitter3, Guanna Li3 (), Chunming Xu1
State Key Laboratory of Heavy Oil Processing, China University of Petroleum (Beijing), Beijing 102249, China
Department of Chemistry, Tsinghua University, Beijing 100084, China
Biobased Chemistry and Technology, Wageningen University & Research, Wageningen, 6708WG, The Netherlands
Department of Materials Science and Engineering, China University of Petroleum (East China), Qingdao 266580, China
Institute of Analysis and Testing, Institute of Analysis and Testing, Beijing Academy of Science and Technology (Beijing Center for Physical and Chemical Analysis), Beijing 100094, China
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Nitrogen-doped carbon supported Fe and Mn heteronuclear single atom catalysts with different Fe and Mn inter-site distance were fabricated for CO2 electroreduction reaction. The catalyst with neighboring Mn and Fe sites showed a CO Faradaic efficiency of 96% at a low overpotential of 320 mV with a Tafel slope of 62 mV·dec−1. The adjacent Mn enhanced the electronic localization of Fe, on which *COOH formation and CO* desorption were boosted.

Abstract

Electrochemical carbon dioxide reduction reaction (CO2RR) into high-value added chemicals and fuels has aroused wide attention, but suffers from high overpotential and poor selectivity. Herein, nitrogen-doped carbon supported Fe and Mn heteronuclear single atom catalysts with different Fe and Mn inter-site distance were fabricated via a templating isolation approach and tested for CO2RR to CO in an aqueous solution. The catalyst with atomically dispersed Fe and Mn sites in close proximity exhibited the highest CO2RR performance, with a CO Faradaic efficiency of 96% at a low overpotential of 320 mV, and a Tafel slope of only 62 mV·dec−1, comparable to state-of-the-art gold catalysts. Experimental analysis combined with theory highlighted that single Mn atom at the neighboring site of Fe enhanced the electronic localization of Fe center, which facilitated the generation of key *COOH intermediate as well as CO* desorption on Fe, leading to superior CO2RR performance at low overpotentials. This work offers atomic-level insights into the correlation between the inter-site distance of atomic sites and CO2RR performance, and paves a new avenue for precise control of single-atom sites on carbon surface for highly active and selective electrocatalysts.

Keywords

CO2 electroreductionheteronuclear single-atom catalystinter-site distanceelectron localizationscaling relationshipslow overpotentials

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Nano Research
Volume 18 Issue 3,
March 2025
Article number: 94907249
DOI: 10.26599/NR.2025.94907249
Cite this article:
Sun X, Zhang B, Lu Q, et al. Tailoring the proximity of iron and manganese atomic sites for efficient CO2 electroreduction reaction. Nano Research, 2025, 18(3): 94907249. https://doi.org/10.26599/NR.2025.94907249
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