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

Qiyang Cheng, Sisi Liu (), Yanzheng He, Mengfan Wang, Haoqing Ji, Yunfei Huan, Tao Qian, Chenglin Yan () and Jianmei Lu ()
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Qiyang Cheng: Soochow University
Sisi Liu: Nantong University
Yanzheng He: Soochow University
Mengfan Wang: Soochow University
Haoqing Ji: Soochow University
Yunfei Huan: Nantong University
Tao Qian: Nantong University
Chenglin Yan: Soochow University
Jianmei Lu: Soochow University

Nature Communications, 2025, vol. 16, issue 1, 1-13

Abstract: 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.

Date: 2025
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DOI: 10.1038/s41467-025-59052-2

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