文献类型：期刊文献

英文题名：Enhanced catalytic performance of transition metal-doped Cr2O3 catalysts for propane dehydrogenation: A microkinetic modeling study

作者：Zhang, Rui[1];Chang, Qing-Yu[1];Ma, Fang[1];Zeeshan, Muhammad[1];Yang, Ming-Lei[1];Sui, Zhi-Jun[1];Chen, De[2];Zhou, Xing-Gui[1];Zhu, Yi-An[1]

机构：[1]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[2]Norwegian Univ Sci & Technol, Dept Chem Engn, N-7491 Trondheim, Norway

年份：2022

卷号：446

外文期刊名：CHEMICAL ENGINEERING JOURNAL

收录：;EI(收录号：20222112142226);WOS:【SCI-EXPANDED(收录号:WOS:000807102100005)】；

基金：Acknowledgements This work is supported by the Natural Science Foundation of China (91645122 and 22073027) and the Natural Science Foundation of Shanghai (20ZR1415800) . The computational time provided by the Notur project is highly acknowledged.

语种：英文

外文关键词：Propane dehydrogenation; Single-atom catalysts; Density functional theory; Microkinetic analysis; Rational catalyst screening

摘要：The catalytic behavior of M1-Cr2O3 (M = Mn-Cu, Ru-Ag, and Os-Au) in propane dehydrogenation (PDH) has been studied by employing microkinetic modeling combined with results from periodic DFT + U calculations. Calculated results indicate that most of the single atoms concerned can be stably present on the Cr2O3 surface. The adsorption energy calculations and Bader charge analysis demonstrate that the acidity of the O sites adjacent to the M sites would be enhanced upon doping, which in turn strengthens the atomic H adsorption and the co adsorption of various PDH species. The surface H formation energy is identified as the reactivity descriptor for PDH over the M1-Cr2O3 catalysts, and a volcano curve of the PDH activity is obtained. By calculating the difference between the propylene dehydrogenation and desorption barriers, it is found that some M1-Cr2O3 catalysts show improved selectivity towards propylene, as compared to Cr2O3. Comparison between the formation barriers of H-2 and H2O reveals that single-atom doping has no apparent negative effect on the catalytic stability of the Cr2O3 surface. The Cu1-Cr(2)O(3 )catalyst is finally identified as the most promising catalyst for PDH among the 13 M-1-Cr2O3 catalyst candidates, considering the catalytic activity, selectivity, stability, and cost.