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Low-temperature fabrication of K2O supported mesoporous tetragonal ZrO2 solid base for synthesis of dimethyl carbonate

Journal 2020 · IF 3.687 · 发表于 2020 年 8 月 9 日
作者: Huahua Zhao,Huanling Song,Fangyuan Wang,Zhichao Miao,Lingjun Chou
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摘要

In the present work, a new strategy was developed to fabricate strong basicity on mesoporous zirconia by in-situ preservation of carbon species originated from organic template during the thermal treatment of mesoporous ZrO 2 . The carbon species was maintained on mesoporous zirconia by calcination in N 2 prior to the introduction of base precursor KNO 3 . The decomposition temperature of KNO 3 to strongly basic site K 2 O was significantly reduced from higher than 650℃ to about 400℃ in the presence of carbon species, which fascinatingly converted the endothermic decomposition reaction to exothermic process. More importantly, the tetragonal ZrO 2 support with excellent mesostructure was well stabilized by the carbon species after introduction of K species. Therefore, K 2 O supported on mesoporous tetragonal zirconia (K 2 O/M-ZrO 2 -C) were successfully fabricated. The resultant mesoporous basic material presented good activity in the synthesis of dimethyl carbonate (DMC) and the DMC yield was 60.0 %, apparently higher than that (18.1 %) of the catalyst prepared without preserving carbon species (K 2 O/M-ZrO 2 ). The strong basicity and the uniform mesopores of the catalyst were suggested to be contributed to the high activity. The obtained results will provide some fundamental understanding and guidance for rational catalyst design.