Controlled proton accessibility through carboxylic-based organic ligands for highly efficient and selective ammonia electrosynthesis

Research output: Journal Publications and ReviewsRGC 21 - Publication in refereed journalpeer-review

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Detail(s)

Original languageEnglish
Article number101024
Journal / PublicationChem Catalysis
Volume4
Issue number7
Online published11 Jun 2024
Publication statusPublished - 18 Jul 2024

Abstract

Competing hydrogen evolution reaction (HER) and sluggish multi-electron/proton-involved steps are the major obstacles to improving the efficiency and selectivity of electrochemical nitrate reduction to ammonia (eNO3RR). Herein, we modified Co3O4 nanoparticles with doped rare-earth La atoms and carboxylic (COO)-based organic ligands. The COO groups efficiently reduce the water activity around the active sites by forming hydrogen bonds, thus controlling proton accessibility and regulating the adsorption selectivity between nitrate ions and protons. Simultaneously, introducing oxygen vacancies through La doping establishes active sites with a strong affinity for nitrate ions and an electron-rich local environment conducive to eNO3RR. The electrocatalyst exhibits superior activity and selectivity with an ammonia Faradaic efficiency of up to 99.41% and a yield rate of 5.62 mg h−1 mgcat−1 at −0.3 V vs. reversible hydrogen electrode (RHE). Notably, the catalyst maintains over 90% Faradaic efficiency for NH3 production across a broad potential range of 400 mV, surpassing most recently reported eNO3RR electrocatalysts. © 2024 Elsevier Inc.

Citation Format(s)

Controlled proton accessibility through carboxylic-based organic ligands for highly efficient and selective ammonia electrosynthesis. / Chen, Dong; Zhang, Shaoce; Yin, Di et al.
In: Chem Catalysis, Vol. 4, No. 7, 101024, 18.07.2024.

Research output: Journal Publications and ReviewsRGC 21 - Publication in refereed journalpeer-review