Mechanical pressure-mediated Pd active sites formation in NaY zeolite catalysts for indirect oxidative carbonylation of methanol to dimethyl carbonate

Wang, Chunzheng; Xu, Ningkun; Liu, Tingting; Xu, Weisong; Guo, Hailing; Li, Yanpeng; Bai, Peng; Wu, Xin‐Ping; Gong, X. G.; Liu, Xinmei; Mintova, Svetlana

doi:10.1016/j.jcat.2021.03.009

Cited by 24 publications

(20 citation statements)

References 72 publications

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“…Thus, the improvement of the DMC production process has drawn much attention. Currently, several main DMC synthesis routes have been developed, including phosgenation, 3 oxidative carbonylation, [4][5][6] alcoholysis of urea, 7,8 transesterification, [9][10][11][12] direct methanol syntheses from CO 2, 13,14 and so on. Among the routes, transesterification represents one of the main carbonate synthesis processes owing to its high atomic utilization, high yield of DMC, and mild reaction conditions (Scheme 1).…”

Section: Introductionmentioning

confidence: 99%

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

et al. 2023

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The application of heterogeneous catalysts in dimethyl carbonate (DMC) synthesis from methanol is hindered by low activation efficiency of methanol to methoxy intermediates (CH3O*), 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 CO2‐TPD, NH3‐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 CH3O* stably, thus synergistically promoted the transesterification. Finally, the CuO/ZnO‐9%K2O 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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Section: Introductionmentioning

confidence: 99%

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

et al. 2023

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“…Thus, the improvement of the DMC production process has drawn much attention. Currently, several main DMC synthesis routes have been developed, including phosgenation 3 , oxidative carbonylation [4][5][6] , alcoholysis of urea 7,8 , transesterification [9][10][11][12] , direct methanol syntheses from CO2 13,14 , and so on. Among the routes, transesterification represents one of the main carbonate synthesis processes owing to its high atomic utilization, high yield of DMC, and mild reaction conditions (Scheme 1).…”

Section: Introductionmentioning

confidence: 99%

K-doped CuO/ZnO with Dual Active Centers of Synergism for Highly Efficient Dimethyl Carbonate Synthesis

Han¹,

Xue²,

Yao³

et al. 2023

Preprint

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The application of heterogeneous catalysts in dimethyl carbonate (DMC) synthesis from methanol is hindered by low activation efficiency of methanol to methoxy intermediates (CH3O*), 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 CO2-TPD, NH3-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 CH3O* stably, thus synergistically promoted the transesterification. Finally, the CuO/ZnO-9%K2O 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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“…As has already been reported, Pd(II) centers favor the DMC product, while Pd(0) active sites preferably produce DMO. 28 In both processes, the Pd active sites are believed to be involved in redox cycles as the reaction processes, that is, a Pd(II)/ Pd(IV) cycle for DMC generation, 18,19,29 and a Pd(0)/Pd(II) cycle for DMO generation. 25,27 The key to selectivity for this reaction, that few previous studies refer to, lies in how the *COOCH 3 intermediates differ from each other in structure or distribution when attached to different surfaces of the catalysts, thus leading to different products.…”

Section: Introductionmentioning

confidence: 99%

Theoretical exploration of the origin of selectivity for the oxidative carbonylation reaction catalyzed by a single Pd atom embedded on graphene

Lin

2023

Catal. Sci. Technol.

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Mechanical pressure-mediated Pd active sites formation in NaY zeolite catalysts for indirect oxidative carbonylation of methanol to dimethyl carbonate

Cited by 24 publications

References 72 publications

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

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

K-doped CuO/ZnO with Dual Active Centers of Synergism for Highly Efficient Dimethyl Carbonate Synthesis

Theoretical exploration of the origin of selectivity for the oxidative carbonylation reaction catalyzed by a single Pd atom embedded on graphene

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