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Intentional corrosion-induced reconstruction of defective NiFe layered double hydroxide boosts electrocatalytic nitrate reduction to ammonia

Nature Water volume 1, pages 1068–1078 (2023)Cite this article

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Abstract

The electroreduction of nitrate to ammonia is particularly important in mitigating environmental pollution and obtaining value-added products. Although non-toxic and inexpensive iron-based materials are expected to be a promising catalyst for electrochemical nitrate reduction, ensuring their sustained high activity and inhibiting spontaneous corrosion requires the implementation of complex design. Here we report an economical self-corrosion approach that utilizes Ni2+ ions in wastewater to control the formation of NiFe layered double hydroxide active phase on iron surface, resulting in high nitrate conversion (97.2%) and ammonia selectivity (90.3%). Coupling nitrate reduction with acid absorption, the conversion from NO3− to (NH4)2SO4(s) for applications such as acting as fertilizer are achieved. This distinctive ‘waste-to-treasure’ perspective not only challenges the conventional belief that corrosion diminishes active phase but also notably improves catalytic efficiency while harnessing valuable resources from wastewater, offering a practical method for converting nitrate to useful ammonia products.

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Fig. 1: Comparison of NO3−RR performance after corrosion of Fe foam in wastewater with or without Ni2+ ions and schematic of NiFe-LDH-Ov growth on Fe surface.
Fig. 2: NO3−-to-NH4+ conversion performance on different cathodes.
Fig. 3: Characterizations analysis.
Fig. 4: Mechanism analysis for enhanced NO3−RR.
Fig. 5: In situ Raman analysis.
Fig. 6: Computational fluid dynamics simulation analysis and ammonia product collection.

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The data supporting the findings in this study are available within the paper (and its Supplementary Information).

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (grant numbers 52270082 (R.M.), 22276210 (X.Z.) and 22106173 (J.Z.)) and Tianjin Science and Technology Program (grant number 22YFYSHZ00270 (R.M.)).

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Authors and Affiliations

  1. State Key Laboratory of Environmental Aquatic Chemistry, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing, People’s Republic of China

    Kaifeng Wang, Ran Mao, Juanjuan Zhang & Xu Zhao

  2. University of Chinese Academy of Sciences, Beijing, People’s Republic of China

    Kaifeng Wang, Ran Mao & Xu Zhao

  3. State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing, People’s Republic of China

    Rui Liu, Huachao Zhao & Wei Ran

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  1. Kaifeng Wang
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Contributions

X.Z. conceived and designed this project and revised this original manuscript. K.W. performed experiments, electrode materials preparation, characterization, data analysis and prepared the manuscript. R.M. contributed to the materials characterizations and experimental data analysis and revised the manuscript. R.L. contributed to discussion and draft editing. J.Z., H.Z. and W.R. discussed the results.

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Correspondence to Xu Zhao.

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Nature Water thanks Jianzhou Gui and Li-Zhi Huang for their contribution to the peer review of this work.

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Wang, K., Mao, R., Liu, R. et al. Intentional corrosion-induced reconstruction of defective NiFe layered double hydroxide boosts electrocatalytic nitrate reduction to ammonia. Nat Water 1, 1068–1078 (2023). https://doi.org/10.1038/s44221-023-00169-3

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