Molecular architectures of iron complexes for oxygen reduction catalysis—Activity enhancement by hydroxide ions coupling

Author:

Ei Phyu Win Poe1,Yang Jiahui1,Ning Shuwang2,Huang Xiang3ORCID,Fu Gengtao2ORCID,Sun Qiming14,Xia Xing-Hua5ORCID,Wang Jiong14ORCID

Affiliation:

1. Innovation Center for Chemical Science, College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou 215006, China

2. Jiangsu Key Laboratory of New Power Batteries, Jiangsu Collaborative Innovation Center of Biomedical Functional Materials, School of Chemistry and Materials Science, Nanjing Normal University, Nanjing 210023, China

3. Department of Physics, Southern University of Science and Technology, Shenzhen 518055, China

4. Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow University, Suzhou, Jiangsu 215123, China

5. State Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China

Abstract

Developing cost-effective and high-performance electrocatalysts for oxygen reduction reaction (ORR) is critical for clean energy generation. Here, we propose an approach to the synthesis of iron phthalocyanine nanotubes (FePc NTs) as a highly active and selective electrocatalyst for ORR. The performance is significantly superior to FePc in randomly aggregated and molecularly dispersed states, as well as the commercial Pt/C catalyst. When FePc NTs are anchored on graphene, the resulting architecture shifts the ORR potentials above the redox potentials of Fe 2+/3+ sites. This does not obey the redox-mediated mechanism operative on conventional FePc with a Fe 2+ –N moiety serving as the active sites. Pourbaix analysis shows that the redox of Fe 2+/3+ sites couples with HO ions transfer, forming a HO–Fe 3+ –N moiety serving as the ORR active sites under the turnover condition. The chemisorption of ORR intermediates is appropriately weakened on the HO–Fe 3+ –N moiety compared to the Fe 2+ –N state and thus is intrinsically more ORR active.

Funder

MOST | National Natural Science Foundation of China

Publisher

Proceedings of the National Academy of Sciences

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