Coexisting Fe single atoms and nanoparticles on hierarchically porous carbon for high-efficiency oxygen reduction reaction and Zn-air batteries

Xiangyu Lu; Yaqiang Li; Derui Dong; Yongbiao Wan; Ruopeng Li; Lihui Xiao; Dan Wang; Lilai Liu; Guangzhao Wang; Jinqiu Zhang; Maozhong An; Peixia Yang

doi:10.1016/j.jcis.2023.09.047

Coexisting Fe single atoms and nanoparticles on hierarchically porous carbon for high-efficiency oxygen reduction reaction and Zn-air batteries

J Colloid Interface Sci. 2024 Jan;653(Pt A):654-663. doi: 10.1016/j.jcis.2023.09.047. Epub 2023 Sep 9.

Authors

Xiangyu Lu¹, Yaqiang Li¹, Derui Dong¹, Yongbiao Wan², Ruopeng Li¹, Lihui Xiao¹, Dan Wang³, Lilai Liu⁴, Guangzhao Wang⁵, Jinqiu Zhang¹, Maozhong An¹, Peixia Yang⁶

Affiliations

¹ MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150001, China.
² Microsystem & Terahertz Research Center, Institute of Electronic Engineering, China Academy of Engineering Physics, Chengdu 610200, China.
³ Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology, School of Petrochemical Engineering, Changzhou University, Changzhou, Jiangsu 213164, China. Electronic address: danwang@cczu.edu.cn.
⁴ College of Environmental and Chemical Engineering, Heilongjiang University of Science and Technology, Harbin 150022, China.
⁵ Key Laboratory of Extraordinary Bond Engineering and Advanced Materials Technology of Chongqing, School of Electronic Information Engineering, Yangtze Normal University, Chongqing 408100, China.
⁶ MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150001, China. Electronic address: yangpeixia@hit.edu.cn.

PMID: 37741173
DOI: 10.1016/j.jcis.2023.09.047

Abstract

Fe single-atom catalysts still suffer from unsatisfactory intrinsic activity and durability for oxygen reduction reaction (ORR). Herein, the coexisting Fe single atoms and nanoparticles on hierarchically porous carbon (denoted as Fe-FeN-C) are prepared via a Zn₅(OH)₆(CO₃)₂-assisted pyrolysis strategy. Theoretical calculation reveals that the Fe nanoparticles can optimize the electronic structures and d-band center of Fe active center, hence reducing the reaction energy barrier for enhancing intrinsic activity. The Zn₅(OH)₆(CO₃)₂ self-sacrificial template not only can promote the formation of Fe single atoms, but also contributes to the construction of microporous/mesoporous/macroporous structures. Therefore, the obtained Fe-FeN-C exhibits impressive ORR activity with a half-wave potential of 0.921 V, which far exceeds Pt/C. With Fe-FeN-C as the cathode catalyst, the assembled Zn-air batteries delivered a maximum power density of 206 mW cm^-2 and a long-cycle life over 400 h.

Keywords: Fe single atoms; Hierarchically porous carbon; Oxygen reduction reaction; Single-atom catalysts; Zn-air batteries.