Design of N-Coordinated Dual-Metal Sites: A Stable and Active Pt-Free Catalyst for Acidic Oxygen Reduction Reaction

Jing Wang; Zhengqing Huang; Wei Liu; Chunran Chang; Haolin Tang; Zhijun Li; Wenxing Chen; Chunjiang Jia; Tao Yao; Shiqiang Wei; Yuen Wu; Yadong Li

doi:10.1021/jacs.7b10385

Design of N-Coordinated Dual-Metal Sites: A Stable and Active Pt-Free Catalyst for Acidic Oxygen Reduction Reaction

J Am Chem Soc. 2017 Dec 6;139(48):17281-17284. doi: 10.1021/jacs.7b10385. Epub 2017 Nov 21.

Authors

Jing Wang¹, Zhengqing Huang², Wei Liu³, Chunran Chang², Haolin Tang⁴, Zhijun Li⁵, Wenxing Chen⁶, Chunjiang Jia⁷, Tao Yao³, Shiqiang Wei³, Yuen Wu¹, Yadong Li⁶

Affiliations

¹ Department of Chemistry, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), University of Science and Technology of China , Hefei 230026, China.
² Institute of Industrial Catalysis, School of Chemical Engineering and Technology, Xi'an Jiaotong University , Xi'an 710049, China.
³ Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China , Hefei 230026, China.
⁴ State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology , Wuhan 430070, China.
⁵ Department of Chemistry, Queen's University , Kingston, Ontario K7L 3N6, Canada.
⁶ Department of Chemistry, Tsinghua University , Beijing 100084, China.
⁷ Key Laboratory for Colloid and Interface Chemistry, Key Laboratory of Special Aggregated Materials, School of Chemistry and Chemical Engineering, Shandong University , Jinan 250100, China.

PMID: 29135246
DOI: 10.1021/jacs.7b10385

Abstract

We develop a host-guest strategy to construct an electrocatalyst with Fe-Co dual sites embedded on N-doped porous carbon and demonstrate its activity for oxygen reduction reaction in acidic electrolyte. Our catalyst exhibits superior oxygen reduction reaction performance, with comparable onset potential (E_onset, 1.06 vs 1.03 V) and half-wave potential (E_1/2, 0.863 vs 0.858 V) than commercial Pt/C. The fuel cell test reveals (Fe,Co)/N-C outperforms most reported Pt-free catalysts in H₂/O₂ and H₂/air. In addition, this cathode catalyst with dual metal sites is stable in a long-term operation with 50 000 cycles for electrode measurement and 100 h for H₂/air single cell operation. Density functional theory calculations reveal the dual sites is favored for activation of O-O, crucial for four-electron oxygen reduction.

Publication types

Research Support, Non-U.S. Gov't