Kuang-Min Zhao, Suqin Liu, Yu-Yang Li, Xianli Wei, Guanying Ye, Weiwei Zhu, Yuke Su, Jue Wang, Hongtao Liu, Zhen He, Zhi-You Zhou, Shi-Gang Sun
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引用次数: 63
Abstract
Identifying the actual structure and tuning the catalytic activity of Fe–N4-based moieties, well-recognized high-activity sites in the oxygen reduction reaction (ORR) are challenging problems. Herein, by using poly(iron phthalocyanine) (PFePc) as an Fe–N4-based model electrocatalyst, a mechanistic insight into the effect of axial ligands on the ORR catalytic activity of Fe–N4 is provided and it is revealed that the ORR activity of Fe–N4 sites with OH desorption as a rate-determining step is related to the energy level gap between the OH pxpy and Fe 3, which can be tuned by regulating the field strength of the axial ligands. Thus, PFePc coordinated with a weak-field ligand I− (PFePc-I) with a low energy level of Fe 3 exhibits high activity evidenced by an ORR half-wave potential as high as 0.948 V versus RHE. This work develops a novel strategy for tuning the ORR activity of Fe–N4 and reveals the correlation between the electronic/geometric structure and catalytic activity of Fe–N4.
期刊介绍:
Established in 2011, Advanced Energy Materials is an international, interdisciplinary, English-language journal that focuses on materials used in energy harvesting, conversion, and storage. It is regarded as a top-quality journal alongside Advanced Materials, Advanced Functional Materials, and Small.
With a 2022 Impact Factor of 27.8, Advanced Energy Materials is considered a prime source for the best energy-related research. The journal covers a wide range of topics in energy-related research, including organic and inorganic photovoltaics, batteries and supercapacitors, fuel cells, hydrogen generation and storage, thermoelectrics, water splitting and photocatalysis, solar fuels and thermosolar power, magnetocalorics, and piezoelectronics.
The readership of Advanced Energy Materials includes materials scientists, chemists, physicists, and engineers in both academia and industry. The journal is indexed in various databases and collections, such as Advanced Technologies & Aerospace Database, FIZ Karlsruhe, INSPEC (IET), Science Citation Index Expanded, Technology Collection, and Web of Science, among others.