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Unveiling the facet-dependent activity of Cu2O for enhanced selective electroreduction of nitric oxide to ammonia and Zn-NO batteries
Process Safety and Environmental Protection ( IF 7.8 ) Pub Date : 2024-05-03 , DOI: 10.1016/j.psep.2024.04.146
Shuang Liu , Linghui Yan , Qi Chen , Bo Wu , Heyang Zhu , Shaodong Zhou , Xiaodan Wang , Xuesong Zhao , Chen Sun , Youzhi Li , Lecheng Lei , Zhongjian Li , Yang Hou , Bin Yang

The conversion of harmful industrial-emitted nitric oxide from emission into valuable NH through NO electrochemical reduction reaction (NORR) is a green and sustainable route, which can enable the nitrogen cycle. However, exploring efficient catalyst and unveiling relevant intrinsic mechanism remains a big challenge for improving the efficiency. Herein, we delve into the facet-dependent activity of CuO nanocrystal, unveiling for the superior performance of oxygen-vacancy-anchored CuO (111) with an unprecedented NH yield of 273.5 μmol h cm and a Faradaic efficiency of 96.9% at −0.4 V vs RHE, which is significantly higher than that of CuO (100) and CuO (100)&(111). CuO (111) with abundant oxygen vacancies and hydroxyl groups facilitated the adsorption of NO and suppressed the hydrogen evolution reaction (HER), insights supported by theoretical calculations and in-situ attenuated total reflectance-surface-enhanced IR absorption spectroscopy (ATR-SEIRAS). Further, leveraging CuO (111) as the cathode, a proof-of-concept Zn-NO battery delivered superior performance with a power density of 4.62 mW cm and an NH yield of 308.0 μg h cm. This work not only elucidates the facet-dependent catalytic behaviors but also sets a new benchmark for NH synthesis and Zn-NO battery development, presenting a significant advancement in the sustainable and efficient conversion of nitric oxide.

中文翻译:

揭示 Cu2O 的晶面依赖性活性,以增强一氧化氮选择性电还原为氨和 Zn-NO 电池

通过NO电化学还原反应(NORR)将有害工业排放的一氧化氮转化为有价值的NH,是一条绿色可持续的途径,可以实现氮循环。然而,探索高效的催化剂并揭示相关的内在机制仍然是提高效率的一大挑战。在此,我们深入研究了 CuO 纳米晶体的晶面依赖性活性,揭示了氧空位锚定的 CuO (111) 的优越性能,其 NH 产量达到前所未有的 273.5 μmol h cm,在 -0.4 V 时法拉第效率为 96.9%与 RHE 相比,显着高于 CuO (100) 和 CuO (100)&(111)。具有丰富氧空位和羟基的 CuO (111) 促进 NO 的吸附并抑制析氢反应 (HER),理论计算和原位衰减全反射表面增强红外吸收光谱 (ATR-SEIRAS) 支持这一见解。此外,利用 CuO (111) 作为阴极,概念验证的 Zn-NO 电池具有卓越的性能,功率密度为 4.62 mW cm,NH 产量为 308.0 μg h cm。这项工作不仅阐明了面依赖的催化行为,而且为NH合成和Zn-NO电池的开发树立了新的基准,在一氧化氮的可持续和高效转化方面取得了重大进展。
更新日期:2024-05-03
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