Nitrogen-doping-induced electron spin polarization activates scandium oxide as high-performance zinc-air battery cathode

Yuhui Chen; Jun Li; Yiqing Chen; Ying Cheng; Xinxin Tian; Dongdong Xiao; Hsiao-Tsu Wang; Ying-Rui Lu; Linjie Zhang; Wenlie Lin; Jun Luo; Lili Han

doi:10.1016/j.jcis.2025.01.223

Nitrogen-doping-induced electron spin polarization activates scandium oxide as high-performance zinc-air battery cathode

J Colloid Interface Sci. 2025 May 15:686:96-106. doi: 10.1016/j.jcis.2025.01.223. Epub 2025 Jan 26.

Authors

Yuhui Chen¹, Jun Li², Yiqing Chen³, Ying Cheng⁴, Xinxin Tian², Dongdong Xiao⁵, Hsiao-Tsu Wang⁶, Ying-Rui Lu⁷, Linjie Zhang⁸, Wenlie Lin⁹, Jun Luo¹⁰, Lili Han¹¹

Affiliations

¹ State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002 China; Institute for New Energy Materials and Low-Carbon Technologies, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin 300384 China.
² State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002 China.
³ Department of Mining and Materials Engineering, McGill University, Montreal, QC H3A0C9, Canada.
⁴ Faculty of Metallurgical and Energy Engineering, Kunming University of Science and Technology, Kunming 650093, China.
⁵ Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China.
⁶ Department of Physics, Tamkang University, New Taipei City 251301, Taiwan.
⁷ National Synchrotron Radiation Research Center, Hsinchu 300092, Taiwan.
⁸ State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002 China. Electronic address: zhanglinjie@fjirsm.ac.cn.
⁹ State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002 China. Electronic address: linwenlie@fjirsm.ac.cn.
¹⁰ ShenSi Lab, Shenzhen Institute for Advanced Study University of Electronic Science and Technology of China, Longhua District, Shenzhen 518110, China.
¹¹ State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002 China. Electronic address: llhan@fjirsm.ac.cn.

PMID: 39892013
DOI: 10.1016/j.jcis.2025.01.223

Abstract

Platinum (Pt) is the most active catalyst for the oxygen reduction reaction (ORR). However, the scarcity, high cost, and susceptibility to deactivation of Pt constrain its large-scale applications. Transition metal oxide (TMO) materials have emerged as promising alternatives due to their abundant availability and catalytic potential. Herein, we report a dissolution-and-carbonization strategy to synthesize a carbon-supported nitrogen-doped Sc₂O₃ catalyst (N-Sc₂O₃/C). Nitrogen doping significantly enhances the conductivity of the otherwise poor-conductivity Sc₂O₃, transforming it into a superior ORR catalyst. The synthesized N-Sc₂O₃/C exhibits remarkable ORR performance in 0.1 M KOH, achieving a half-wave potential of 0.92 V, which is 55 mV higher than the state-of-the-art commercial Pt/C (0.87 V). Moreover, as a cathode for a zinc-air battery, N-Sc₂O₃/C achieves a peak power density of 150.7 mW cm^-2 and a specific capacity of 766.4 mAh g_Zn^-1. Density functional theory calculations reveal that nitrogen doping induces electron spin polarization within Sc₂O₃, narrowing the bandgap. This enhanced electronic structure improves conductivity and optimizes the adsorption of oxygen intermediates, thereby facilitating the ORR process. Our study demonstrates that nitrogen doping activates the wide-bandgap Sc₂O₃ semiconductor, converting it into a highly efficient ORR electrocatalyst and highlighting the potential of wide-bandgap TMO materials in energy applications.

Keywords: Nitrogen doping; Oxygen reduction reaction; Scandium oxide; Transition metal oxide; Zinc-air battery.