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Metal-nitrogen-carbon (M-N-C) single-atom catalysts exhibit desirable electrochemical catalytic properties. However, the replacement of N atoms by heteroatoms (B, P, S, etc.) has been regarded as a useful method for regulating the coordination environment. The structure engineered M-N-C sites via doping heteroatoms play an important role to the adsorption and activation of the oxygen intermediate. Herein, we develop an efficient strategy to construct dual atomic site catalysts via the formation of a Co1-PN and Ni1-PN planar configuration. The developed Co1-PNC/Ni1-PNC catalyst exhibits excellent bifunctional electrocatalytic performance in alkaline solution. Both experimental and theoretical results demonstrated that the N/P coordinated Co/Ni sites moderately reduced the binding interaction of oxygen intermediates. The Co1-PNC/Ni1-PNC endows a rechargeable Zn-air battery with excellent power density and cycling stability as an air-cathode, which is superior to that of the benchmark Pt/C+IrO2. This work paves an avenue for design of dual single-atomic sites and regulation of the atomic configuration on carbon-based materials to achieve high-performance electrocatalysts.
This work was supported by the National Natural Science Foundation of China (Nos. 21971135, 21925202, 21872076, and 21590792), the National Key R&D Program of China (Nos. 2017YFA0700101 and 2016YFA0202801), and Beijing Natural Science Foundation (No. JQ18007). We thank the 1W1B station for XAFS measurement in Beijing Synchrotron Radiation Facility (BSRF). Professor Yitai Qian, one of the pioneers of the inorganic chemistry in China, has made a great contribution in the fields of inorganic synthesis chemistry and superconducting materials. We benefit from his words and deeds. This article is dedicated to Professor Yitai Qian on the occasion of his 80th birthday.