A highly CO-tolerant atomically dispersed Pt catalyst for chemoselective hydrogenation
A highly CO-tolerant atomically dispersed Pt catalyst for chemoselective hydrogenation
复制标题
DOI：
10.1038/s41565-019-0366-5
复制
发表时间：
2019-04-01
影响因子：
38.3
通讯作者：
Ma, Ding
中科院分区：
文献类型：
--
作者：
Lin, Lili;Yao, Siyu;Ma, Ding
贵金属，特别是铂催化剂的加氢活性很容易被反应原料中微量一氧化碳的存在所抑制。开发具有高活性和选择性的抗co加氢催化剂具有重要的经济意义，因为它可以使用廉价的粗氢，避免昂贵的产物分离。在这里，我们证明了原子分散的铂在α -碳化钼（α - moc）上构成了一种高度抗co的催化剂，用于硝基苯衍生物的化学选择性加氢。Pt-1/ α - moc催化剂在5000 ppm CO的存在下表现出良好的活性，并且对硝基加氢具有很强的化学特异性。在水的辅助下，以CO和水作为氢源，在不牺牲选择性和稳定性的情况下，也可以实现高的加氢活性。缺乏电子的铂单原子上CO结合的减弱和硝基加氢的新反应途径使催化剂具有较高的CO电阻率和化学选择性。
The hydrogenation activity of noble metal, especially platinum (Pt), catalysts can be easily inhibited by the presence of a trace amount of carbon monoxide (CO) in the reaction feeds. Developing CO-resistant hydrogenation catalysts with both high activity and selectivity is of great economic interest for industry as it allows the use of cheap crude hydrogen and avoids costly product separation. Here we show that atomically dispersed Pt over alpha-molybdenum carbide (alpha-MoC) constitutes a highly CO-resistant catalyst for the chemoselective hydrogenation of nitrobenzene derivatives. The Pt-1/alpha-MoC catalyst shows promising activity in the presence of 5,000 ppm CO, and has a strong chemospecificity towards the hydrogenation of nitro groups. With the assistance of water, high hydrogenation activity can also be achieved using CO and water as a hydrogen source, without sacrificing selectivity and stability. The weakened CO binding over the electron-deficient Pt single atom and a new reaction pathway for nitro group hydrogenation confer high CO resistivity and chemoselectivity on the catalyst.