Accelerating Industrial-Level NO3 Electroreduction to Ammonia on Cu Grain Boundary Sites via Heteroatom Doping Strategy

Yan Wang, Shuai Xia, Rui Cai, Jianfang Zhang*, Jiarui Wang, Cuiping Yu, Jiewu Cui, Yong Zhang, Jingjie Wu, Shize Yang, Hark Hoe Tan, Yucheng Wu*

*Corresponding author for this work

    Research output: Contribution to journalArticlepeer-review

    12 Citations (Scopus)

    Abstract

    Although the electrocatalytic nitrate reduction reaction (NO3RR) is an attractive NH3 synthesis route, it suffers from low yield due to the lack of efficient catalysts. Here, this work reports a novel grain boundary (GB)-rich Sn-Cu catalyst, derived from in situ electroreduction of Sn-doped CuO nanoflower, for effectively electrochemical converting NO3 to NH3. The optimized Sn1%-Cu electrode achieves a high NH3 yield rate of 1.98 mmol h−1 cm−2 with an industrial-level current density of −425 mA cm−2 at −0.55 V versus a reversible hydrogen electrode (RHE) and a maximum Faradaic efficiency of 98.2% at −0.51 V versus RHE, outperforming the pure Cu electrode. In situ Raman and attenuated total reflection Fourier transform infrared spectroscopies reveal the reaction pathway of NO3RR to NH3 by monitoring the adsorption property of reaction intermediates. Density functional theory calculations clarify that the high-density GB active sites and the competitive hydrogen evolution reaction (HER) suppression induced by Sn doping synergistically promote highly active and selective NH3 synthesis from NO3RR. This work paves an avenue for efficient NH3 synthesis over Cu catalyst by in situ reconstruction of GB sites with heteroatom doping.

    Original languageEnglish
    Article number2302295
    JournalSmall
    Volume19
    Issue number26
    DOIs
    Publication statusPublished - 28 Jun 2023

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