Nitrogen-Doped Carbon Polyhedrons Confined Fe-P Nanocrystals as High-Efficiency Bifunctional Catalysts for Aqueous Zn-CO2 Batteries

Shuai Liu; Lei Wang; Hui Yang; Sanshuang Gao; Yifan Liu; Shusheng Zhang; Yu Chen; Xijun Liu; Jun Luo

doi:10.1002/smll.202104965

Nitrogen-Doped Carbon Polyhedrons Confined Fe-P Nanocrystals as High-Efficiency Bifunctional Catalysts for Aqueous Zn-CO₂ Batteries

Small. 2022 Mar;18(10):e2104965. doi: 10.1002/smll.202104965. Epub 2022 Jan 15.

Authors

Shuai Liu¹, Lei Wang², Hui Yang³, Sanshuang Gao¹, Yifan Liu⁴, Shusheng Zhang⁵, Yu Chen², Xijun Liu^{1

6}, Jun Luo¹

Affiliations

¹ Institute for New Energy Materials and Low-Carbon Technologies, Tianjin Key Lab for Photoelectric Materials and Devices, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin, 300384, China.
² Tianjin Key Laboratory of Organic Solar Cells and Photochemical Conversion, Tianjin Key Laboratory of Drug Targeting and Bioimaging, School of Chemistry and Chemical Engineering, Tianjin University of Technology, Tianjin, 300384, China.
³ School of Materials Science and Engineering, Tianjin University of Technology, Tianjin, 300384, China.
⁴ College of Physics and Optoelectronic Engineering, Shenzhen University, Shenzhen, 518060, China.
⁵ College of Chemistry, Zhengzhou University, Zhengzhou, 450000, China.
⁶ MOE Key Laboratory of New Processing Technology for Non-Ferrous Metals and Materials, and Guangxi Key Laboratory of Processing for Non-Ferrous Metals and Featured Materials, School of Resource, Environments and Materials, Guangxi University, Nanning, 530004, China.

PMID: 35032144
DOI: 10.1002/smll.202104965

Abstract

Emerging Fe bonded with heteroatom P in carbon matrix (FePC) holds great promise for electrochemical catalysis, but the design of highly active and cost-efficient FePC structure for the electrocatalytic CO₂ reduction reaction (CO₂ RR) and aqueous ZnCO₂ batteries (ZCBs) is still challenging. Herein, polyhedron-shaped bifunctional electrocatalysts, FeP nanocrystals anchored in N-doped carbon polyhedrons (Fe-P@NCPs), toward a reversible aqueous ZnCO₂ battery, are reported. The Fe-P@NCPs are synthesized through a facile strategy by using self-templated zeolitic imidazolate frameworks (ZIFs), followed by an in situ high-temperature calcination. The resultant catalysts exhibit aqueous CO₂ RR activity with a CO Faradaic efficiency up to 95% at -0.55 V versus reversible hydrogen electrode (RHE), comparable to the previously best-reported values of FeNC structure. The as-constructed ZCBs with designed Fe-P@NCPs cathode, show the peak power density of 0.85 mW cm^-2 and energy density of 231.8 Wh kg^-1 with a cycling durability over 500 cycles, and outstanding stability in terms of discharge voltage for 7 days. The high selectivity and efficiency of the battery are attributed to the presence of highly catalytic FeP nanocrystals in N-doped carbon matrix, which can effectively increase the number of catalytically active sites and interfacial charge-transfer conductivity, thereby improving the CO₂ RR activity.

Keywords: Fe P nanocrystals; Zn CO 2 batteries; carbon dioxide electrolysis; carbon neutral cycle; metal-organic frameworks-derived carbon.

Abstract

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