Chinese Journal of Catalysis ( IF 15.7 ) Pub Date : 2023-06-22 , DOI: 10.1016/s1872-2067(23)64439-0
Xinjie Song , Shipeng Fan , Zehua Cai , Zhou Yang , Xun Chen , Xianzhi Fu , Wenxin Dai
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A photothermal catalytic system comprising Cu/CeO2 was applied to the reaction between NO, CO and H2O for the production of NH3 under visible-light irradiation. High NO conversion (94.4%) and NH3 selectivity (66.5%) were achieved over Cu/CeO2 in the presence of H2O at 210 °C. Visible light further improved the conversion of NO (97.7%) and selectivity for NH3 (69.1%). The quasi-situ EPR and in-situ DRIFTS results indicated that CO initially reacts with H2O to form an HCO3* intermediate, which then decomposes into CO2 and activated H*. Finally, NO reacts with activated H* to produce NH3. The localized surface plasmon resonance effect of Cu nanoparticles induced by visible light promotes the decomposition of HCO3* to CO2 and H*, while regenerating oxygen vacancies (OVs, H2O activation sites) at the CeO2 sites, resulting in enhanced NH3 production. This study offers a convenient approach for NH3 production under mild conditions.
中文翻译:

在 Cu/CeO2 上存在 H2O 的情况下,通过可见光辅助热催化 CO 还原 NO 合成 NH3
将Cu/CeO 2光热催化体系应用于可见光照射下NO、CO和H 2 O反应生成NH 3 。在 210 °C的 H 2 O存在下,与 Cu/CeO 2相比,实现了高 NO 转化率 (94.4%) 和 NH 3选择性 (66.5%)。可见光进一步提高了NO的转化率(97.7%)和NH 3的选择性(69.1%)。准原位EPR和原位DRIFTS结果表明CO最初与H 2 O反应形成HCO 3 *中间体,然后分解为CO 2并激活H*。最后,NO与活化的H*反应生成NH 3 。可见光诱导的Cu纳米颗粒的局域表面等离子体共振效应促进HCO 3 *分解为CO 2和H*,同时在CeO 2位点再生氧空位(OV、H 2 O活化位点) ,从而增强NH 3生产。本研究为在温和条件下生产NH 3提供了一种便捷的方法。