Palladium containing EMT zeolite catalyst(Pd/EMT) was prepared and used for the indirect oxidative carbonylation of methanol to dimethyl carbonate(DMC).The EMT zeolite was employed as a new catalyst support and compar...Palladium containing EMT zeolite catalyst(Pd/EMT) was prepared and used for the indirect oxidative carbonylation of methanol to dimethyl carbonate(DMC).The EMT zeolite was employed as a new catalyst support and compared with the conventional Pd containing FAU zeolite catalyst(Pd/FAU).The Pd/EMT in contrast to the Pd/FAU catalyst exhibited high intrinsic activity with the turnover frequency of 0.25 s^(-1) vs.0.11 s^(-1).The Pd/EMT catalyst showed high CO conversion of 82% and DMC selectivity of 79%,that maintained for at least 130 h,while the activity of the Pd/FAU catalyst rapidly deteriorated within 12 h.The enhanced interactions between Pd and EMT zeolite inhibited the sintering of palladium clusters and maintained the Pd2+ active sites in the Pd/EMT catalyst.The stabilization of the mono-dispersed Pd clusters within the EMT zeolite is paramount to the excellent performance of the catalyst for the indirect oxidative carbonylation of methanol to DMC.展开更多
基金supported by the National Natural Science Foundation of China (21908246, 21975285, U1862118)China Postdoctoral Science Foundation (2017M622311)+1 种基金Fundamental Research Funds for the Central Universities (18CX02148A)the Sino-French International Laboratory (LIA) “Zeolites”。
文摘Palladium containing EMT zeolite catalyst(Pd/EMT) was prepared and used for the indirect oxidative carbonylation of methanol to dimethyl carbonate(DMC).The EMT zeolite was employed as a new catalyst support and compared with the conventional Pd containing FAU zeolite catalyst(Pd/FAU).The Pd/EMT in contrast to the Pd/FAU catalyst exhibited high intrinsic activity with the turnover frequency of 0.25 s^(-1) vs.0.11 s^(-1).The Pd/EMT catalyst showed high CO conversion of 82% and DMC selectivity of 79%,that maintained for at least 130 h,while the activity of the Pd/FAU catalyst rapidly deteriorated within 12 h.The enhanced interactions between Pd and EMT zeolite inhibited the sintering of palladium clusters and maintained the Pd2+ active sites in the Pd/EMT catalyst.The stabilization of the mono-dispersed Pd clusters within the EMT zeolite is paramount to the excellent performance of the catalyst for the indirect oxidative carbonylation of methanol to DMC.
基金financially supported by the National Key R&D Program of China (2022YFA1503400)the National Natural Science Foundation of China (21991091)+2 种基金the Key Projects of Shandong Key R&D plan (2019JZZY010506)Taishan Scholar Foundation (tspd20210308)the Petro China Research and Development Projects (2020A-1816 and 2020A-1817)。
