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K-doped CuO/ZnO with dual active centers of synergism for highly efficient dimethyl carbonate synthesis

Journal 2023 · IF 3.7 · 69(10): e18158 · 发表于 2023 年 6 月 15 日
作者: Han Han,Xue Ye,Jie Yao,Xinhua Gao,Jinghao Yu,Lisheng Guo,Jie Li
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摘要

The application of heterogeneous catalysts in dimethyl carbonate (DMC) synthesis from methanol is hindered by low activation efficiency of methanol to methoxy intermediates (CH 3 O*), which is the key intermediate for DMC generation. Herein, a catalyst of alkali metal K anchored on the CuO/ZnO oxide is rationally designed for offering Lewis acid–base pairs as dual active centers to improve the activation efficiency of methanol. Characterizations of CO 2 -TPD, NH 3 -TPD, XPS, and DRIFTS revealed that the addition of Lewis base K observably boosted the dissociation of methanol and combined with Lewis acid CuO/ZnO oxide to adsorb the formed CH 3 O* stably, thus synergistically promoted the transesterification. Finally, the CuO/ZnO-9%K 2 O catalyst exhibited the optimal catalytic activity, achieving a high yield of 74.4% with an excellent selectivity of 98.9% for DMC at a low temperature of 90°C. The strategy of constructing Lewis acid–base pairs provides a reference for the design of heterogeneous catalysts.

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