Electron-rich Au nanocrystals/Co3O4 interface for enhanced electrochemical nitrate reduction into ammonia

文献类型： 外文期刊

第一作者： Zhang, Maolin

作者： Zhang, Maolin;He, Wen-Qing;Liu, Jialei;Liu, Chen;Huang, Hao;Song, Kepeng;Zhang, Zedong

作者机构： Chinese Acad Agr Sci, Inst Environm & Sustainable Dev Agr, Beijing 100081, Peoples R China;King Abdullah Univ Sci & Technol, Div Phys Sci & Engn, Thuwal 239556900, Saudi Arabia;Shandong Univ, Electron Microscopy Ctr, Jinan 250100, Peoples R China;Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China

关键词： Electron transfer; Interface; Nitrate reduction; Solar-driven

期刊名称：JOURNAL OF COLLOID AND INTERFACE SCIENCE （ 2022影响因子：9.9； 五年影响因子：8.4 ）

ISSN： 0021-9797

年卷期： 2023 年 650 卷

页码：

收录情况： SCI

摘要： Solar-driven electrochemical NO3 - reduction reaction (NO3-RR) is a clean and sustainable strategy that can convert pollutant NO3 - in wastewater to value-added NH3. In recent years, cobalt oxides-based catalysts have shown their intrinsic catalytic properties toward NO3-RR but still have room for improvement through catalyst design. Coupling metal oxides with noble metal has been demonstrated to improve electrochemical catalytic efficiency. Here, we use Au species to tune the surface structure of Co3O4 and improve the efficiency of NO3-RR to NH3. The obtained Au nanocrystals-Co3O4 catalyst exhibited an onset potential of 0.54 V vs RHE, NH3 yield rate of 27.86 & mu;g/h & BULL;cm2, and Faradaic efficiency (FE) of 83.1% at 0.437 V vs RHE in an H-cell, which is much higher than Au small species (Au clusters or single atoms)-Co3O4 (15.12 & mu;g/h & BULL;cm2) and pure Co3O4 (11.38 & mu;g/h & BULL;cm2), respectively. Combined experiments with theory calculations, we attributed the enhanced performance of Au nanocrystals-Co3O4 to the reduced energy barrier of *NO hydrogenation to the *NHO and suppression of HER, which originated from the charge transfer from Au to Co3O4. Using an amorphous silicon triple-junction (a-Si TJ) as the solar cell and an anion exchange membrane electrolyzer (AME), an unassisted solar-driven NO3-RR to NH3 prototype was realized with a yield rate of 4.65 mg/h and FE of 92.1%.

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