Directional Manipulation of Electron Transfer by Energy Level Engineering for Efficient Cathodic Oxygen Reduction

作者：Yang Wang, Tianpei Zhou, Shanshan Ruan, Feng Hu, Wentuan Bi, Jun Hu, Ting Chen, Hongfei Liu, Bingkai Yuan, Nan Zhang, Wenjie Wang, Lidong Zhang, Wangsheng Chu, Changzheng Wu, Yi Xie · 发表于：Nano Letters · 年份：2022 · DOI：10.1021/acs.nanolett.2c01933 · 被引用次数：42 · 研究领域：Electrocatalysts for Energy Conversion、CO2 Reduction Techniques and Catalysts、Advanced battery technologies research

Electron transfer plays an important role in determining the energy conversion efficiency of energy devices. Nitrogen-coordinated single metal sites (M-N 4 ) materials as electrocatalysts have exhibited great potential in devices. However, there are still great difficulties in how to directionally manipulate electron transfer in M-N 4 catalysts for higher efficiency. Herein, we demonstrated the mechanism of electron transfer being affected by energy level structure based on classical iron phthalocyanine (FePc) molecule/carbon models and proposed an energy level engineering strategy to manipulate electron transfer, preparing high-performance ORR catalysts. Engineering molecular energy level via modulating FePc molecular structure with nitro induces a strong interfacial electronic coupling and efficient charge transfer from carbon to FePc-β-NO 2 molecule. Consequently, the assembled zinc-air battery exhibits ultrahigh performance which is superior to most of M-N 4 catalysts. Energy level engineering provides a universal approach for directionally manipulating electron transfer, bringing a new concept to design efficient and stable M-N 4 electrocatalyst.