Highly Selective, Facile NO2 Reduction to NO at Cryogenic Temperatures on Hydrogen Precovered Gold

详细信息    查看全文

• 作者：Ming Pan ; Hyung Chul Ham ; Wen-Yueh Yu ; Gyeong S. Hwang ; C. Buddie Mullins
• 刊名：The Journal of the American Chemical Society
• 出版年：2013
• 出版时间：January 9, 2013
• 年：2013
• 卷：135
• 期：1
• 页码：436-442
• 全文大小：405K
• 年卷期：v.135,no.1(January 9, 2013)
• ISSN：1520-5126

文摘

We have discovered that NO₂ is reduced to NO at 77 K by hydrogen precovered gold in vacuum. Here, we investigate the partial reduction of NO₂ to NO on an atomic-hydrogen populated model gold catalyst for a more fundamental understanding of the surface chemistry of hydrogenation. Gold-based catalysts have been found to be active for many hydrogenation reactions, but few related fundamental studies have been conducted. Our experimental results reveal a high catalytic activity for gold: indeed, NO₂ is reduced to NO with 100% conversion and 100% selectivity at temperatures lower than 120 K. Density functional theory calculations and reflection鈥揳bsorption infrared spectroscopy measurements indicate that HNO₂ and N₂O₃ are intermediates which are highly dependent on surface hydrogen concentrations; subsequent hydrogenation of HNO₂ and dissociation of N₂O₃ upon annealing induces the production of NO and H₂O.