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Multivariate covalent organic frameworks with tailored electrostatic potential promote nitrate electroreduction to ammonia in acid.

Created on 20 Apr 2025

Authors

Qiyang Cheng, Sisi Liu, Yanzheng He, Mengfan Wang, Haoqing Ji, Yunfei Huan, Tao Qian, Chenglin Yan, Jianmei Lu

Published in

Nature communications. Volume 16. Issue 1. Pages 3717. Apr 19, 2025. Epub Apr 19, 2025.

Abstract

The direct synthesis of ammonia from nitrate (NO3-) reduction in acid is a promising approach for industrialization. However, the difficulty arises from the intense competition with the inevitable hydrogen evolution reaction, which is favoured due to the overwhelming protons (H+). Here, we systematically explore and rationally optimize the microenvironment using multivariate covalent organic frameworks (COFs) as catalyst adlayers to promote the nitrate-to-ammonia conversion in acid. With the application of tailored positive electrostatic potential generated over the multivariate COFs, both the mass transfer of NO3- and H+ are regulated via appropriate electrostatic interactions, thus realizing the priority of NO3RR with respect to HER or NO3--to-NO2-. As a result, an NH3 yield rate of 11.01 mmol h-1 mg-1 and a corresponding Faradaic efficiency of 91.0% are attained, and solid NH4Cl with a high purity of 96.2% is directly collected in acid; therefore, this method provides a practical approach for economically valorising wastewater into valuable ammonia.

PMID:
40253373
Bibliographic data and abstract were imported from PubMed on 20 Apr 2025.

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