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Activity and stability of titanosilicate supported Au catalyst for propylene epoxidation with H2 and O2
Molecular Catalysis ( IF 4.6 ) Pub Date : 2018-02-08 , DOI: 10.1016/j.mcat.2018.01.039
Sainan Yao , Luhang Xu , Jing Wang , Xiaoliang Jing , Tareque Odoom-Wubah , Daohua Sun , Jiale Huang , Qingbiao Li

Highly dispersed Au catalysts supported on amorphous titanosilicate supports with three-dimensional wormhole-like mesoporosity were prepared by deposition–precipitation method, which show excellent performance in propylene epoxidation with H2 and O2. The best catalytic performance, propylene conversion of 12.8%, propylene oxide selectivity of 76.2% and PO space-time yield of 160.9 gpo/Kgcat/h, was obtained at the reaction temperature of 300 °C. The Ti/Si molar ratio of the supports and some experimental parameters, such as the urea amount, loading temperature and Au loading on the as-produced catalyst are optimized. In addition, with the assistance of in-situ Fourier transform infrared spectroscopy (In-situ FT-IR), adsorption and desorption of PO, propylene and the reaction mixture on the catalyst are conducted to further explore the deactivation mechanism. It suggests that propylene and PO can be irreversibly and strongly adsorbed on the catalyst surface and finally transform to carbonate adsorbed on the active sites Ti-OH, resulting in catalyst deactivation.



中文翻译:

钛硅酸盐负载的Au催化剂对H 2和O 2进行丙烯环氧化的活性和稳定性

采用沉积-沉淀法制备了具有三维蠕虫状介孔结构的非晶态钛硅酸盐载体上高分散的Au催化剂,该催化剂在H 2和O 2的丙烯环氧化反应中表现出优异的性能。在300°C的反应温度下获得了最佳的催化性能,丙烯转化率为12.8%,环氧丙烷选择性为76.2%,PO时空产率为160.9 g po / Kg cat / h。优化了载体的Ti / Si摩尔比和一些实验参数,如尿素用量,负载温度和Au负载量。此外,借助原位傅里叶变换红外光谱仪(进行了原位FT-IR,对PO,丙烯以及反应混合物在催化剂上的吸附和解吸,以进一步探讨其失活机理。这表明丙烯和PO不可逆地强烈吸附在催化剂表面,最终转变为吸附在活性位Ti-OH上的碳酸盐,导致催化剂失活。

更新日期:2018-02-08
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