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

Ei Phyu Win，Poe1; Yang，Jiahui1; Ning，Shuwang2; Huang，Xiang3; Fu，Gengtao2; Sun，Qiming1,4; Xia，Xing Hua5; Wang，Jiong1,4

2024-03-12

10.1073/pnas.2316553121

Proceedings of the National Academy of Sciences of the United States of America   影响因子和分区

1091-6490

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 Fe2+/3+ sites. This does not obey the redox-mediated mechanism operative on conventional FePc with a Fe2+-N moiety serving as the active sites. Pourbaix analysis shows that the redox of Fe2+/3+ sites couples with HO- ions transfer, forming a HO-Fe3+-N moiety serving as the ORR active sites under the turnover condition. The chemisorption of ORR intermediates is appropriately weakened on the HO-Fe3+-N moiety compared to the Fe2+-N state and thus is intrinsically more ORR active.

collective effects molecular assembly molecular electrochemistry oxygen reduction reaction redox-mediated mechanism

SCI

英语

其他

BIOLOGY & BIOCHEMISTRY ; CLINICAL MEDICINE ; MULTIDISCIPLINARY ; PLANT & ANIMAL SCIENCE ; ENVIRONMENT/ECOLOGY ; SOCIAL SCIENCES, GENERAL ; MICROBIOLOGY ; ECONOMICS BUSINESS ; IMMUNOLOGY ; MATERIALS SCIENCE ; MATHEMATICS ; SPACE SCIENCE ; MOLECULAR BIOLOGY & GENETICS ; PHARMACOLOGY & TOXICOLOGY ; CHEMISTRY ; PSYCHIATRY/PSYCHOLOGY ; NEUROSCIENCE & BEHAVIOR ; PHYSICS ; GEOSCIENCES ; AGRICULTURAL SCIENCES ; ENGINEERING

2-s2.0-85186847004

Scopus

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,215123,China
5.State Key Laboratory of Analytical Chemistry for Life Science,School of Chemistry and Chemical Engineering,Nanjing University,Nanjing,210023,China

Ei Phyu Win，Poe,Yang，Jiahui,Ning，Shuwang,et al. Molecular architectures of iron complexes for oxygen reduction catalysis-Activity enhancement by hydroxide ions coupling[J]. Proceedings of the National Academy of Sciences of the United States of America,2024,121(11).

Ei Phyu Win，Poe.,Yang，Jiahui.,Ning，Shuwang.,Huang，Xiang.,Fu，Gengtao.,...&Wang，Jiong.(2024).Molecular architectures of iron complexes for oxygen reduction catalysis-Activity enhancement by hydroxide ions coupling.Proceedings of the National Academy of Sciences of the United States of America,121(11).

Ei Phyu Win，Poe,et al."Molecular architectures of iron complexes for oxygen reduction catalysis-Activity enhancement by hydroxide ions coupling".Proceedings of the National Academy of Sciences of the United States of America 121.11(2024).