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用于高效电催化硝酸盐还原的RuO-CoO纳米颗粒的界面介导电子结构调控

The interface-mediated electron structure tuning of RuO-CoO nano-particles for efficient electrocatalytic nitrate reduction.

作者信息

Liu Yang, Jiang Xiaoli, Zhang Yagang, Li Hangqi, Huang Weidong, Yang Yuanteng, Ye Minghao, Liu Yanxia

机构信息

School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu 611731, China.

State Key Laboratory of Electronic Thin Films and Integrated Devices, University of Electronic Science and Technology of China, Chengdu 611731, China.

出版信息

Dalton Trans. 2023 Dec 19;53(1):162-170. doi: 10.1039/d3dt03318j.

DOI:10.1039/d3dt03318j
PMID:38018516
Abstract

The energy-intensive processes for the industrial production of ammonia necessitates the development of new methods to be proposed that will aid in reducing the global energy consumption. Specifically, the electrocatalytic nitrate reduction reaction (NORR) to produce ammonia is more thermodynamically feasible than the electrocatalytic nitrogen reduction reaction (NRR). However, it is hindered by a low catalytic activity due to its complex reaction pathways. Herein, we synthesized a novel electrocatalyst, RuO-CoO nanoparticles, with abundant interfaces, which exhibited an enhanced catalytic activity for efficient ammonia synthesis. This catalyst delivered a partial current density of 65.8 mA cm for NH production, a faradaic efficiency (FE) of 89.7%, and a superior ammonia yield rate of up to 210.5 μmol h cm at -0.6 V RHE. X-ray photoelectron and Raman spectroscopy revealed that the formed interfacial Ru-O-Co bond can decorate the electronic structures of the active sites and accelerate the absorption of NO, thus promoting the production of ammonia.

摘要

氨的工业生产中能源密集型工艺需要提出新方法,以帮助降低全球能源消耗。具体而言,电催化硝酸盐还原反应(NORR)制氨比电催化氮还原反应(NRR)在热力学上更可行。然而,由于其复杂的反应路径,该反应受到低催化活性的阻碍。在此,我们合成了一种具有丰富界面的新型电催化剂RuO-CoO纳米颗粒,其对高效氨合成表现出增强的催化活性。该催化剂在-0.6 V(相对于可逆氢电极,RHE)下产生NH的部分电流密度为65.8 mA cm,法拉第效率(FE)为89.7%,氨产率高达210.5 μmol h cm。X射线光电子能谱和拉曼光谱表明,形成的界面Ru-O-Co键可以修饰活性位点的电子结构并加速NO的吸附,从而促进氨的生成。

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