Solvent environment engineering to synthesize FeNC nanocubes with densely Fe-Nx sites as oxygen reduction catalysts for Zn-air battery

Hao Xu; Lihui Xiao; Peixia Yang; Xiangyu Lu; Lilai Liu; Dan Wang; Jinqiu Zhang; Maozhong An

doi:10.1016/j.jcis.2023.01.140

Solvent environment engineering to synthesize FeNC nanocubes with densely Fe-N_x sites as oxygen reduction catalysts for Zn-air battery

J Colloid Interface Sci. 2023 May 15:638:242-251. doi: 10.1016/j.jcis.2023.01.140. Epub 2023 Jan 31.

Authors

Hao Xu¹, Lihui Xiao¹, Peixia Yang², Xiangyu Lu¹, Lilai Liu³, Dan Wang⁴, Jinqiu Zhang¹, Maozhong An¹

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, 150001 Harbin, China.
² MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, 150001 Harbin, China. Electronic address: yangpeixia@hit.edu.cn.
³ College of Environmental and Chemical Engineering, Heilongjiang University of Science and Technology, 150022 Harbin, China.
⁴ Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology, School of Petrochemical Engineering, Changzhou University, 213164 Changzhou, China.

PMID: 36738547
DOI: 10.1016/j.jcis.2023.01.140

Abstract

Zeolitic imidazole framework (ZIF)-derived iron-nitrogen-carbon (FeNC) materials are expected to be high-efficiency catalysts for oxygen reduction reaction (ORR). However, increasing the density of active sites while avoiding metal accumulation still faces significant challenges. Herein, solvent environment engineering is used to synthesize the FeNC containing dense Fe-N_x moieties by adjusting the solvent during the ZIF precursor synthesis process. Compared with methanol and water/methanol, the aqueous media can provide a more moderate Fe content for the ZIF precursor, which facilitates the construction of high-density Fe-N_x sites and prevent the appearance of iron-based nanoparticles during pyrolysis. Therefore, the FeNC(C) nanocubes synthesized in an aqueous media have the highest single atom Fe loading (0.6 at%) among the prepared samples, which presents excellent oxygen reduction properties and durability under alkaline and acidic conditions. The advantage of FeNC(C) is proven in Zn-air batteries, with outstanding performance and long-term stability.

Keywords: Active site loading; Oxygen reduction reaction; Single-atom Fe-N(x); Solvent environment engineering; Zeolitic imidazole framework.

MeSH terms

Iron
Methanol*
Oxygen
Solvents
Water
Zeolites*
Zinc

Substances

Solvents
Methanol
Water
Iron
Zeolites
Oxygen
Zinc