H₂O₂-mediated electrosynthesis of nitrate from air

Date

2024

Authors

Dong, K.
Yao, Y.
Li, H.
Li, H.
Sun, S.
He, X.
Wang, Y.
Luo, Y.
Zheng, D.
Liu, Q.

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Nature Synthesis, 2024; 3(6):763-773

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Kai Dong, Yongchao Yao, Haobo Li, Huangjingwei Li, Shengjun Sun, Xun He, Yan Wang, Yongsong Luo, Dongdong Zheng, Qian Liu, Quan Li, Dongwei Ma, Xuping Sun, Bo Tang

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Abstract

Renewable electricity-driven electrochemical nitrogen oxidation is a promising alternative to traditional Haber–Bosch and Ostwald processes to directly synthesize nitrate from nitrogen. However, its efficiency is hindered by strong competition from the oxygen evolution reaction in aqueous environments, along with a deficiency in standardized testing protocols. Here we present an efficient approach for nitrogen oxidation, substituting the oxygen evolution reaction with hydroxyl radicals (·OH) generated through hydrogen peroxide decomposition to serve as an active oxygen source. Electrochemical tests demonstrate that the nitrogen oxidation, facilitated by ·OH, can achieve a Faradaic efficiency of 25.6% and a nitrate yield of 8.3 nmol s−1 cm−2. Furthermore, we employed in situ electrochemical mass spectrometry, gas-phase infrared and electron paramagnetic resonance spectroscopy to establish a comprehensive set of benchmarks to confirm the authenticity of nitrogen activation and to examine the reaction mechanism mediated by ·OH. Techno-economic analysis underscores the promising feasibility and sustainable economic value of the presented method.

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© The Author(s), under exclusive licence to Springer Nature Limited 2024. Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.

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