Preparation of MeCeOx(Me=In, Zr) Solid Solution Catalyst for the Application in the Synthesis of Dimethyl Carbonate

Abstract

Abstract: MeCeO_x (Me=In, Zr) bimetallic oxide catalysts were prepared by liquid-phase co-precipitation method with a matrix of CeO₂. The physiochemical properties of MeCeO_x were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), temperature programmed reduction(H₂-TPR), temperature programmed desorption(CO₂-TPD, CH₃OH-TPD), and diffuse reflectance infrared fourier transform spectroscopy (DRIFTS) techniques. Based on the systematic investigation of the types and doping amounts of various metal oxides, the structure properties and catalytic behavior of solid solution catalysts prepared by doping CeO₂ with different metal oxides were comparatively studied in this paper. The results show that the solid solution structure formed by MeCeO_x bimetal oxide catalysts increases the concentration of oxygen vacancy defects. The InCeO_x solid solution catalyst exhibit the largest concentration of oxygen vacancy defects, resulting in the improve chemical adsorption for CO₂ and CH₃OH molecules. Under the condition of reaction pressure 1.0 MPa, reaction temperature 140 ℃, reaction space velocity (GHSV) 3 600 mL/(g·h) and V(CO₂)/V(CH₃OH)/V(N₂)=4∶1∶5, the InCeO_x shows the excellent catalytic performance with dimethyl carbonate selectivity of 91.3%, CH₃OH conversion of 8.4%, and dimethyl carbonate STY(Space Time Yield) of 0.11 g_DMC·h^-1·g^-1_cat. In addition, further in-depth DRIFTS study show that activation of CO₂ with oxygen vacancies and the formation of terminal methoxy as the intermediate are the crucial to the enhance selectivity of dimethyl carbonate.

Key words: InCeO_x catalyst, bimetallic oxide, solid solution structure, oxygen vacancy, dimethyl carbonate

CLC Number:

O643.3

WANG Yizhou, LIU Fei, ZHAO Tianxiang, CAO Jianxin, XU Fang. Preparation of MeCeO_x(Me=In, Zr) Solid Solution Catalyst for the Application in the Synthesis of Dimethyl Carbonate[J]. Journal of Synthetic Crystals, 2021, 50(1): 113-121.

References

[1] GIBSON D H. Carbon dioxide coordination chemistry: metal complexes and surface-bound species. What relationships?[J]. Coordination Chemistry Reviews, 1999, 185: 335-355.
[2] JACOBSON M Z. Review of solutions to global warming, air pollution, and energy security[J]. Energy Environ Sci, 2009, 2(2): 148-173.
[3] ARESTA M, DIBENEDETTO A, ANGELINI A. Catalysis for the valorization of exhaust carbon: from CO₂ to chemicals, materials, and fuels. Technological use of CO₂[J]. Chemical reviews, 2014, 114(3): 1709-1742.
[4] ONO Y. Catalysis in the production and reactions of dimethyl carbonate, an environmentally benign building block[J]. Applied Catalysis A General, 1997, 155(2): 133-166.
[5] ONO Y. Dimethyl carbonate for environmentally benign reactions[J]. Catalysis Today, 1997, 35(1/2): 15-25.
[6] KELLER N, REBMANN G, KELLER V. Catalysts, mechanisms and industrial processes for the dimethylcarbonate synthesis[J]. Journal of Molecular Catalysis A: Chemical, 2010, 317(1/2): 1-18.
[7] KING S T. Reaction mechanism of oxidative carbonylation of methanol to dimethyl carbonate in Cu-Y zeolite[J]. Journal of Catalysis, 1996, 161(2): 530-538.
[8] TATSUMI T, WATANABE Y, KOYANO K A. Synthesis of dimethyl carbonate from ethylene carbonate and methanol using TS-1 as solid base catalyst[J]. Chemical Communications, 1996(19): 2281.
[9] DELLEDONNE D, RIVETTI F, ROMANO U. Developments in the production and application of dimethylcarbonate[J]. Applied Catalysis A: General, 2001, 221(1/2): 241-251.
[10] TOMISHIGE K, SAKAIHORI T, IKEDA Y, et al. A novel method of direct synthesis of dimethyl carbonate from methanol and carbon dioxide catalyzed by zirconia[J]. Catalysis Letters, 1999, 58(4): 225-229.
[11] BIAN J, XIAO M, WANG S J, et al. Highly effective synthesis of dimethyl carbonate from methanol and carbon dioxide using a novel copper-nickel/graphite bimetallic nanocomposite catalyst[J]. Chemical Engineering Journal, 2009, 147(2/3): 287-296.
[12] CHEN H L, WANG S J, Xiao M, et al. Direct synthesis of dimethyl carbonate from CO₂ and CH₃OH using 0.4 nm molecular sieve supported Cu-Ni Bimetal catalyst[J]. Chinese Journal of Chemical Engineering, 2012, 20(5): 906-913.
[13] ZHOU Y J, WANG S J, XIAO M, et al. Novel Cu-Fe bimetal catalyst for the formation of dimethyl carbonate from carbon dioxide and methanol[J]. RSC Advances, 2012, 2(17): 6831-6837.
[14] ARESTA M, DIBENEDETTO A, PASTORE C, et al. Cerium(IV)oxide modification by inclusion of a hetero-atom: a strategy for producing efficient and robust nano-catalysts for methanol carboxylation[J]. Catalysis Today, 2008, 137(1): 125-131.
[15] KANG K H, LEE C H, KIM D B, et al. NiO/CeO₂-ZnO nano-catalysts for direct synthesis of dimethyl carbonate from methanol and carbon dioxide[J]. Journal of Nanoscience and Nanotechnology, 2014, 14(11): 8693-8698.
[16] ZHANG M, XIAO M, WANG S J, et al. Cerium oxide-based catalysts made by template-precipitation for the dimethyl carbonate synthesis from carbon dioxide and methanol[J]. Journal of Cleaner Production, 2015, 103: 847-853.
[17] KUMAR P, WITH P,SRIVASTAVA V C, et al. Dimethyl carbonate synthesis from carbon dioxide using ceria-zirconia catalysts prepared using a templating method: characterization, parametric optimization and chemical equilibrium modeling[J]. RSC Advances,2016,6(111): 110235-110246.
[18] LI A X, PU Y F, LI F, et al. Synthesis of dimethyl carbonate from methanol and CO₂ over Fe-Zr mixed oxides[J]. Journal of CO₂ Utilization, 2017, 19: 33-39.
[19] FU Z Z, ZHONG Y Y, YU Y H, et al. TiO₂-doped CeO₂ nanorod catalyst for direct conversion of CO₂ and CH₃OH to dimethyl carbonate: catalytic performance and kinetic study[J]. ACS Omega, 2018, 3(1): 198-207.
[20] STOIAN D, MEDINA F, URAKAWA A. Improving the stability of CeO₂ catalyst by rare earth metal promotion and molecular insights in the dimethyl carbonate synthesis from CO₂ and methanol with 2-cyanopyridine[J]. ACS Catalysis, 2018, 8(4): 3181-3193.
[21] CHEN Y D, WANG H, QIN Z X, et al. Ti_xCe_1-xO₂ nanocomposites: a monolithic catalyst for the direct conversion of carbon dioxide and methanol to dimethyl carbonate[J]. Green Chemistry, 2019, 21(17): 4642-4649.
[22] SCHMITT R, NENNING A, KRAYNIS O, et al. A review of defect structure and chemistry in ceria and its solid solutions[J]. Chemical Society Reviews, 2020, 49(2): 554-592.
[23] YE J Y, LIU C J, MEI D H, et al. Active oxygen vacancy site for methanol synthesis from CO₂ hydrogenation on In₂O₃(110):a DFT study[J]. ACS Catalysis, 2013, 3(6): 1296-1306
[24] WANG J J, TANG C Z, LI G N, et al. High performance MaZrO_x (Ma=Cd, Ga) solid solution catalysts for CO₂ hydrogenation to methanol[J]. ACS Catalysis, 2019, 9(11): 10253-10259.
[25] CHEN T Y, CAO C, CHEN T, et al. Unraveling highly tunable selectivity in CO₂ hydrogenation over bimetallic In-Zr oxide catalysts[J]. ACS Catalysis, 2019, 9(9): 8785-8797.
[26] LIU B, LI C M, ZHANG G Q. Oxygen vacancy promoting dimethyl carbonate synthesis from CO₂and methanol over Zr-doped CeO₂ nanorods[J]. ACS Catalysis, 2018, 8(11): 10446-10456.

Preparation of MeCeO_x(Me=In, Zr) Solid Solution Catalyst for the Application in the Synthesis of Dimethyl Carbonate

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