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Efficient Nitrate Synthesis via Ambient Nitrogen Oxidation with Ru-Doped TiO2 /RuO2 Electrocatalysts.
Advanced Materials ( IF 27.4 ) Pub Date : 2020-05-25 , DOI: 10.1002/adma.202002189
Min Kuang 1 , Yu Wang 2, 3 , Wei Fang 1 , Huiteng Tan 1 , Mengxin Chen 1 , Jiandong Yao 1 , Chuntai Liu 4 , Jianwei Xu 5 , Kun Zhou 2, 3 , Qingyu Yan 1
Affiliation  

A facile pathway of the electrocatalytic nitrogen oxidation reaction (NOR) to nitrate is proposed, and Ru‐doped TiO2/RuO2 (abbreviated as Ru/TiO2) as a proof‐of‐concept catalyst is employed accordingly. Density functional theory (DFT) calculations suggest that Ruδ + can function as the main active center for the NOR process. Remarkably doping Ru into the TiO2 lattice can induce an upshift of the d‐band center of the Ru site, resulting in enhanced activity for accelerating electrochemical conversion of inert N2 to active NO*. Overdoping of Ru ions will lead to the formation of additional RuO2 on the TiO2 surface, which provides oxygen evolution reaction (OER) active sites for promoting the redox transformation of the NO* intermediate to nitrate. However, too much RuO2 in the catalyst is detrimental to both the selectivity of the NOR and the Faradaic efficiency due to the dominant OER process. Experimentally, a considerable nitrate yield rate of 161.9 µmol h−1 gcat−1 (besides, a total nitrate yield of 47.9 µg during 50 h) and a highest nitrate Faradaic efficiency of 26.1% are achieved by the Ru/TiO2 catalyst (with the hybrid composition of Rux Tiy O2 and extra RuO2 by 2.79 wt% Ru addition amount) in 0.1 m Na2SO4 electrolyte.

中文翻译:

Ru掺杂的TiO2 / RuO2电催化剂通过环境氮氧化有效合成硝酸盐。

提出了电催化氮氧化反应(NO)转化为硝酸盐的简便途径,并相应地采用Ru掺杂的TiO 2 / RuO 2(缩写为Ru / TiO 2)作为概念验证催化剂。密度泛函理论(DFT)计算表明,钌δ +罐功能作为主要活性中心为NOR过程。将Ru显着地掺杂到TiO 2晶格中可以引起Ru位点d谱带中心的上移,从而增强了活性,以促进惰性N 2电化学转化为活性NO *。Ru离子的过量掺杂将导致在TiO 2上形成额外的RuO 2表面,该表面提供了氧气释放反应(OER)活性位,以促进NO *中间体氧化还原转化为硝酸盐。然而,由于占主导地位的OER工艺,催化剂中的RuO 2过多对NOR的选择性和法拉第效率都不利。实验上,通过Ru / TiO 2催化剂,硝酸盐的产率很高,为161.9 µmol h -1 g cat -1(此外,在50小时内硝酸盐总产量为47.9 µg),硝酸法拉第效率最高(26.1%)(在0.1 m内具有Ru x Ti y O 2和多余的RuO 2的混合组成,Ru添加量为2.79 wt% Na 2 SO 4电解质。
更新日期:2020-07-01
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