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Oxygen vacancy engineering of calcium cobaltate: A nitrogen fixation electrocatalyst at ambient condition in neutral electrolyte

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Abstract

In order to sustainably transform N2 to ammonia (NRR) using electrocatalysts under mild ambient condition, it is urgent to design and develop non-nobel metal nanocatalysts that are inexpensive and suitable for mass-production. Herein, a calcium metalate catalyst CaCoOx with oxygen vacancies was synthesized and used as an electrocatalyst for NRR for the first time, whose morphology can be controlled by the calcination temperature and the heating rate. Under the optimal conditions, the CaCoOx catalyst achieved the yield of nitrogen conversion to ammonia of 16.25 µg·h−1·mgcat−1 at the potential of −0.3 V relative to the reversible hydrogen electrode (RHE) with a Faraday efficiency of 20.51%. The electrocatalyst showed good stability even after 12 times recyclability under environmental conditions and neutral electrolyte. Later, the electrocatalytic nitrogen reduction performance of CaFeOx, CaNiOx, CaCuOx was investigated. These earth-rich transition metals also exhibited certain NRR electrocatalytic capabilities, which provided a door for further development of inexpensive and easily available transition metal as nitrogen reduction electrocatalysts.

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Acknowledgements

The authors gratefully acknowledge the financial support from the National Natural Science Foundation of China (Nos. 21871042, 21471028 and 21671036), Changbai Mountain Scholarship, Natural Science Foundation of Jilin Province (No. 20200201083JC), and Natural Science Foundation of Department of education of Jilin Province (No. JJKH20201169KJ).

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  1. **nyu Chen and Ke Li contributed equally to this work.

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  1. Key Laboratory of Polyoxometalate Science of the Ministry of Education, Faculty of Chemistry, Northeast Normal University, Changchun, 130024, China

    **nyu Chen, Ke Li, **aoxuan Yang, Jiaqi Lv, Sai Sun, Siqi Li, Dongming Cheng, Bo Li, Yang-Guang Li & Hong-Ying Zang

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  1. **nyu Chen
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Oxygen vacancy engineering of calcium cobaltate: A nitrogen fixation electrocatalyst at ambient condition in neutral electrolyte

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Chen, X., Li, K., Yang, X. et al. Oxygen vacancy engineering of calcium cobaltate: A nitrogen fixation electrocatalyst at ambient condition in neutral electrolyte. Nano Res. 14, 501–506 (2021). https://doi.org/10.1007/s12274-020-3043-y

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