Experimental and theoretical investigations into propane dehydrogenation over MIL-101(Cr/Al) derived catalysts

Propane dehydrogenation is commonly operated at temperatures exceeding 600 °C due to thermodynamic requirements. However, high temperature accelerates the deactivation of catalysts because of the coke deposition. Therefore, it is quite necessary to develop catalysts with high catalytic activity and improved anti-coking ability. To this end, an Al-doped Cr2O3 catalyst derived from MIL-101(Cr/Al) is prepared in this work. The preparation conditions, including the carbonization temperature of MIL-101 and the proportion of Cr/Al, are optimized via experimental studies. Meanwhile, the adsorption and dehydrogenation behaviors of propane on the catalyst are investigated using Density Functional Theory (DFT) methods. Findings indicate that the optimum carbonization temperature and Cr/Al proportion are 900 °C and 6:4, respectively. Under the reaction condition of P = 0.1 MPa, T = 580 °C and GHSV = 800 h−1, the propane conversion and propylene selectivity on the Cr6/Al4 catalyst are 19.5% and 92.0%, respectively. The activity stability of the Al-doped Cr2O3 is elongated significantly due to the lower desorption energy of propene and higher energy barrier for the coke formation on the catalyst. In sum, the present work completed via experiments and DFT calculations will lead to a better understanding of the Al-doped Cr2O3 catalyst and guide the rational design of anti-coking catalysts for propane dehydrogenation.