脱氢
丙烷
氢化物
催化作用
锌
化学
选择性
光化学
无机化学
有机化学
氢
作者
Shaojia Song,Kun Yang,Peng Zhang,Wu Zhi,Jun Li,Hui Su,Sheng Dai,Chunming Xu,Zhenxing Li,Jian Liu,Weiyu Song
标识
DOI:10.1021/acscatal.2c00928
摘要
Propane dehydrogenation (PDH) is promising for producing high value-added propylene. The discovery of a more efficient, economical, and nontoxic PDH catalyst is of great importance. Herein, we found zinc hydrides ([ZnH]+) as the highly reactive site for PDH. In situ spectroscopy and theoretical studies reveal that [ZnH]+ was transformed from zinc hydroxyl ([ZnOH]+) sites under reductive conditions. Accordingly, the formation of [ZnH]+ can be controlled by adjusting the amount of zinc hydroxyl ([ZnOH]+) species by various additives. The optimized Cu–ZnO@S-1 consists of exclusively isolated [ZnOH]+ sites, which help produce more [ZnH]+ toward optimal PDH activity. Specifically, the catalyst enables 43% propane conversion with >88% propylene selectivity, close to the thermodynamic equilibrium. This efficient PDH performance was attributed to the electron-deficient Zn in [ZnH]+ that can lower the dehydrogenation barrier, and the Cu-modified [ZnH]+ structure favors the direct PDH pathway to further promote the formation of propylene and H2.
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