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Anion leaching induced amorphous Cu/CuOx on N-doped carbon for efficient electrochemical nitrate reduction to ammonia

文献类型： 外文期刊

作者： Zhang, Maolin 2 ; Peramaiah, Karthik 3 ; Yi, Moyu 4 ; Huang, Hao 1 ;

作者机构： 1.Univ Sci & Technol China, Nano Sci & Technol Inst, Suzhou Inst Adv Res, Suzhou 215123, Peoples R China

2.Chinese Acad Agr Sci, Inst Environm & Sustainable Dev Agr, Beijing 100081, Peoples R China

3.Agcy Sci Technol Res & ASTAR, Inst Sustainabil Chem Energy & Environm ISCE2, Singapore 627833, Singapore

4.King Abdullah Univ Sci & Technol, Ctr Renewable Energy & Storage Technol CREST, Chem Program, Div Phys Sci & Engn, Thuwal 239556900, Saudi Arabia

期刊名称：JOURNAL OF MATERIALS CHEMISTRY A （ 影响因子：9.5； 五年影响因子：10.3 ）

ISSN： 2050-7488

年卷期： 2025 年 13 卷 32 期

页码：

收录情况： SCI

摘要： The electrochemical valorization of nitrate-containing industrial wastewater into green ammonia (NH3) presents a carbon-neutral pathway for simultaneously addressing environmental remediation and sustainable chemical production. Copper-based catalysts exhibit inherent advantages in the nitrate reduction reaction (NtRR) due to their optimal d-band electronic structure for *NO3- adsorption/activation. However, their performance is fundamentally constrained by insufficient active site density. Herein, we propose an anion leaching-driven dynamic reconstruction strategy to engineer self-optimizing Cu/CuOx heterostructured catalysts through chronoamperometric activation of CuCl-decorated nitrogen-doped carbon black (CuCl-N/CB). Spectroscopic characterization studies reveal that potential-induced Cl- leaching triggers structural reconstruction, creating abundant dual-active Cu0-Cu+ sites for the NtRR. The resulting amorphous Cu/CuOx-N/CB reveals the highest NH3 yield rate of 6.94 mg cm-2 h-1 with a faradaic efficiency (FE) of 92.4% at -0.76 V vs. RHE, which are 1.20 and 1.21 times higher than those of the directly prepared Cu-N/CB catalyst in terms of NH3 yield rate and FE, respectively. Scaling to proton-exchange membrane (PEM) electrolyzers demonstrates industrial relevance, delivering 68.11 mg h-1 NH3 production at 96.8% FE under 88.7 mA cm-2. This work provides an effective strategy to prepare Cu-based catalysts from CuX (X = Cl, Br, or I), which show high activity and NH3 selectivity in the NtRR.

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