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锚定在氮掺杂碳纳米管上的异质结构Co/CoO作为硝酸盐还原制氨的高效电催化剂。

Heterostructured Co/CoO anchored on N-doped carbon nanotubes as a highly efficient electrocatalyst for nitrate reduction to ammonia.

作者信息

He Xianxian, Liu Hongfei, Qin Jiangzhou, Niu Zhaodong, Mu Jincheng, Liu Baojun

机构信息

College of Resource and Environmental Engineering, Guizhou University, Guiyang 550025, China.

Department of Environmental Engineering, Peking University, The Key Laboratory of Water and Sediment Sciences, Ministry of Education, Beijing 100871, China.

出版信息

Dalton Trans. 2023 Aug 8;52(31):10869-10875. doi: 10.1039/d3dt01705b.

Abstract

The electrochemical reduction of nitrate (NO) to ammonia (NH) has emerged as an attractive approach for selectively reducing NO to highly value-added NH and removing NO pollutants simultaneously. In this work, a heterostructured Co/CoO electrocatalyst anchored on N-doped carbon nanotubes was prepared and applied for the NO reduction towards NH under alkaline conditions. The catalyst achieves outstanding performance with up to 67% NH faradaic efficiency at -1.2 V Hg/HgO and 8.319 mg h mg yield at -1.7 V Hg/HgO. In addition, it also exhibits good long-term stability. N isotopic labelling experiments prove that the yielded NH is derived from NO species. electrochemical Raman spectra revealed that the structure of the as-prepared catalyst showed outstanding stability and identified possible intermediates during the electrocatalytic NO reduction reaction (NORR).

摘要

将硝酸盐(NO)电化学还原为氨(NH₃)已成为一种有吸引力的方法,可将NO选择性还原为高附加值的NH₃,同时去除NO污染物。在这项工作中,制备了一种锚定在氮掺杂碳纳米管上的异质结构Co/CoO电催化剂,并将其应用于碱性条件下NO还原为NH₃的反应。该催化剂表现出优异的性能,在-1.2 V(相对于Hg/HgO)时NH₃的法拉第效率高达67%,在-1.7 V(相对于Hg/HgO)时产率为8.319 mg h⁻¹ mg⁻¹。此外,它还表现出良好的长期稳定性。N同位素标记实验证明生成的NH₃来源于NO物种。电化学拉曼光谱表明,所制备催化剂的结构表现出优异的稳定性,并确定了电催化NO还原反应(NORR)过程中可能的中间体。

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