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Au Nanowires Decorated Ultrathin Co3O4 Nanosheets toward Light-Enhanced Nitrate Electroreduction
Small ( IF 13.0 ) Pub Date : 2023-03-27 , DOI: 10.1002/smll.202300530 Ze-Nong Zhang 1 , Qing-Ling Hong 2 , Xiao-Hui Wang 1 , Hao Huang 3 , Shu-Ni Li 1 , Yu Chen 2
Small ( IF 13.0 ) Pub Date : 2023-03-27 , DOI: 10.1002/smll.202300530 Ze-Nong Zhang 1 , Qing-Ling Hong 2 , Xiao-Hui Wang 1 , Hao Huang 3 , Shu-Ni Li 1 , Yu Chen 2
Affiliation
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Nitrate is a reasonable alternative instead of nitrogen for ammonia production due to the low bond energy, large water-solubility, and high chemical polarity for good absorption. Nitrate electroreduction reaction (NO3RR) is an effective and green strategy for both nitrate treatment and ammonia production. As an electrochemical reaction, the NO3RR requires an efficient electrocatalyst for achieving high activity and selectivity. Inspired by the enhancement effect of heterostructure on electrocatalysis, Au nanowires decorated ultrathin Co3O4 nanosheets (Co3O4-NS/Au-NWs) nanohybrids are proposed for improving the efficiency of nitrate-to-ammonia electroreduction. Theoretical calculation reveals that Au heteroatoms can effectively adjust the electron structure of Co active centers and reduce the energy barrier of the determining step (*NO → *NOH) during NO3RR. As the result, the Co3O4-NS/Au-NWs nanohybrids achieve an outstanding catalytic performance with high yield rate (2.661 mg h−1 mgcat−1) toward nitrate-to-ammonia. Importantly, the Co3O4-NS/Au-NWs nanohybrids show an obviously plasmon-promoted activity for NO3RR due to the localized surface plasmon resonance (LSPR) property of Au-NWs, which can achieve an enhanced NH3 yield rate of 4.045 mg h−1 mgcat−1. This study reveals the structure–activity relationship of heterostructure and LSPR-promotion effect toward NO3RR, which provide an efficient nitrate-to-ammonia reduction with high efficiency.
中文翻译：
金纳米线装饰超薄 Co3O4 纳米片用于光增强硝酸盐电还原
硝酸盐由于其低键能、大水溶性和高化学极性以利于吸收，是替代氮气用于氨生产的合理替代品。硝酸盐电还原反应（NO 3 RR）是硝酸盐处理和氨生产的有效且绿色的策略。作为一种电化学反应，NO 3 RR 需要高效的电催化剂来实现高活性和选择性。受异质结构对电催化增强作用的启发，Au纳米线装饰超薄Co 3 O 4纳米片（Co 3 O 4-NS/Au-NWs）纳米杂化物被提议用于提高硝酸盐到氨的电还原效率。理论计算表明，Au杂原子可以有效调节Co活性中心的电子结构，降低NO 3 RR过程中决定步骤(*NO→*NOH)的能垒。结果，Co 3 O 4 -NS/Au-NWs纳米杂化物实现了对硝酸盐到氨的优异催化性能和高收率（2.661 mg h -1 mg cat -1 ）。重要的是，Co 3 O 4 -NS/Au-NWs 纳米杂化物对 NO 3显示出明显的等离子体促进活性由于Au-NWs的局域表面等离子体共振（LSPR）特性而产生的RR，可以实现4.045 mg h -1 mg cat -1的增强的NH 3产率。这项研究揭示了异质结构的构效关系和局域表面等离子体共振对 NO 3 RR 的促进作用，从而实现了高效的硝酸盐还原为氨。
更新日期：2023-03-27
中文翻译：
金纳米线装饰超薄 Co3O4 纳米片用于光增强硝酸盐电还原
硝酸盐由于其低键能、大水溶性和高化学极性以利于吸收，是替代氮气用于氨生产的合理替代品。硝酸盐电还原反应（NO 3 RR）是硝酸盐处理和氨生产的有效且绿色的策略。作为一种电化学反应，NO 3 RR 需要高效的电催化剂来实现高活性和选择性。受异质结构对电催化增强作用的启发，Au纳米线装饰超薄Co 3 O 4纳米片（Co 3 O 4-NS/Au-NWs）纳米杂化物被提议用于提高硝酸盐到氨的电还原效率。理论计算表明，Au杂原子可以有效调节Co活性中心的电子结构，降低NO 3 RR过程中决定步骤(*NO→*NOH)的能垒。结果，Co 3 O 4 -NS/Au-NWs纳米杂化物实现了对硝酸盐到氨的优异催化性能和高收率（2.661 mg h -1 mg cat -1 ）。重要的是，Co 3 O 4 -NS/Au-NWs 纳米杂化物对 NO 3显示出明显的等离子体促进活性由于Au-NWs的局域表面等离子体共振（LSPR）特性而产生的RR，可以实现4.045 mg h -1 mg cat -1的增强的NH 3产率。这项研究揭示了异质结构的构效关系和局域表面等离子体共振对 NO 3 RR 的促进作用，从而实现了高效的硝酸盐还原为氨。
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