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Efficient nitrite-to-ammonia electroreduction over Zr-Ni frustrated Lewis acid-base pairs

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Abstract

Electrochemical NO2−-to-NH3 conversion (NO2RR) offers a green route to NH3 electrosynthesis, while developing efficient NO2RR catalysis systems at high current densities remains a grand challenge. Herein, we report an efficient Zr-NiO catalyst with atomically dispersed Zr-dopants incorporated in NiO lattice, delivering the exceptional NO2RR performance with industrial-level current density (>0.2 A cm−2). In situ spectroscopic measurements and theoretical simulations reveal the construction of Zr-Ni frustrated Lewis acid-base pairs (FLPs) on Zr-NiO, which can substantially increase the number of absorbed nitrite (NO2−), promote the activation and protonation of NO2− and concurrently hamper the H coverage, boosting the activity and selectivity of Zr-NiO towards the NO2RR. Remarkably, Zr-NiO exhibits the exceptional performance in a flow cell with high Faradaic efficiency for NH3 of 94.0% and NH3 yield rate of 1,394.1 µmol h−1 cm−2 at an industrial-level current density of 228.2 mA cm−2, placing it among the best NO2RR electrocatalysts for NH3 production.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (52161025) and the Natural Science Foundation of Gansu Province (20JR10RA241).

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Authors and Affiliations

  1. School of Materials Science and Engineering, Lanzhou Jiaotong University, Lanzhou, 730070, China

    Ying Zhang, Zhuohang Li, Wenyu Du, Kai Chen & Ke Chu

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  1. Ying Zhang
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  2. Zhuohang Li
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  3. Wenyu Du
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  4. Kai Chen
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  5. Ke Chu
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Correspondence to Ke Chu.

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Supporting information The supporting information is available online at http://chem.scichina.com and http://link.springer.com/journal/11426. The supporting materials are published as submitted, without typesetting or editing. The responsibility for scientific accuracy and content remains entirely with the authors.

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Zhang, Y., Li, Z., Du, W. et al. Efficient nitrite-to-ammonia electroreduction over Zr-Ni frustrated Lewis acid-base pairs. Sci. China Chem. 67, 1707–1714 (2024). https://doi.org/10.1007/s11426-023-1924-7

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  • DOI: https://doi.org/10.1007/s11426-023-1924-7

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