AIChE Journal, Vol.62, No.11, 3963-3972, 2016
Au/TS-1 catalyst for propene epoxidation with H-2/O-2: A novel strategy to enhance stability by tuning charging sequence
For propene epoxidation with H-2 and O-2, the catalytic performance of Au/TS-1 catalyst is extremely sensitive to preparation parameters of deposition-precipitation (DP) method. In this work, effect of charging sequence in DP process on catalyst structure and catalytic performance of Au/TS-1 catalyst is first investigated. For different charging sequences, the compositions of Au complexes (e.g., [AuCl(OH)(3)](-)) and pore property of TS-1 (i.e., with or without H2O prefilling micropores) could affect the transfer of Au complexes into the micropores, resulting in different Au locations and thus significantly different catalytic performance. Notably, when TS-1 is first filled with H2O and then mixed with Au complexes, the reduced Au/TS-1 catalyst could expose Au nanoparticles on the external surface of TS-1 and show high stability. The results provide direct evidence showing that micropore blocking is the deactivation mechanism. Based on the results, a simple strategy to design highly stable Au/Ti-based catalysts is developed. (c) 2016 American Institute of Chemical Engineers AIChE J, 62: 3963-3972, 2016
Keywords:propene epoxidation;deposition-precipitation method;charging sequence;Au location;catalytic stability