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Catalytic activity of Cu/ZnO catalysts mediated by MgO promoter in hydrogenation of methyl acetate to ethanol

Journal of Energy Chemistry 2021年第10期30卷 203-209,I0006页

作者： Fang Zhang Zhiyang Chen Xudong Fang Hongchao Liu Yong Liu Wenliang Zhu National Engineering Laboratory for Methanol to Olefins Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina Dalian National Laboratory for Clean Energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China

Hydrogenation of methyl acetate is a key step in ethanol synthesis from dimethyl ether carbonylation and Cu-based catalysts are widely *** report here that the hydrogenation activity of Cu/ZnO catalysts can be enhanced by the addition of MgO *** evolution of crystal phases during coprecipitation and the physicochemical properties of calcined and reduced catalysts by X-ray diffraction(XRD),thermogravimetric(TG)-mass spectrometry(MS),Brunauer-Emmett-Teller(BET),transmission electron microscopy(TEM),N_(2)O titration,in situ CO-Fourier transform infrared spectroscopy(FTIR)and H_(2)-temperature programmed reduction(H_(2)-TPR)reveal that the promoter effect likely lies in the presence of Mg^(2+).A proper amount of Mg^(2+)mediates the precipitation process of Cu and Zn,leading to preferable formation of aurichalcite(Cu_(x)Zn_(1-x))5(CO_(3))_(2)(OH)_(6) crystal phase and a small amount of basic carbonates such as hydrozincite Zn_(5)(CO_(3))_(2)(OH)_(6) and malachite Cu_(2) CO_(3)(OH)_(2).The presence of aurichalcite strengthens the interaction between Cu and Zn species,and thus enhances the dispersity of CuO species and helps generation of Cu^(+)species on reduced ***,the performance of Cu/ZnO catalysts exhibits an optimal dependence on the Mg loading,i.e.,17.5%.However,too much Mg^(2+)in the precipitation liquid prohibits formation of aurichalcite but enhances formation of basic nitrates,leading to a dramatically reduced hydrogenation *** findings may find applications for optimization of other Cu-based catalysts in a wider range of hydrogenation reactions.

关键词： Methyl acetate Hydrogenation Cu/ZnO catalyst MgO promoter Precursor effect aurichalcite

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A Modified Co-precipitation Method to Prepare Cu/ZnO/Al2O3 Catalyst and Its Application in Low Temperature Water-gas Shift(LT-WGS)Reaction

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Journal of Wuhan University of Technology(Materials Science) 2018年第4期33卷 876-883页

作者：许龙龙 PENG Dong LIU Wenhui FENG Yimin HOU Yanan LI Xiongjian 黄驰 Tianhua Chemical Branch Xi'an Sunward Aeromat Co.Ltd.Xi'an 710065China Sanjiang Chemical Factory of CSSG Yuanan 444200China College of Chemistry and Molecular Scienees Wuhan UniversityWuhan 430072China

A modified co-precipitation method for the production of Cu/ZnO/Al2O3 complex was studied. The modification was that part of Al was introduced by adding Al^（3＋） into Cu^（2＋）/Zn^（2＋） solution, and the rest of Al was added after co-precipitation step in the form of pseudo-boehmite. The prepared samples were characterized by different techniques such as X-ray diffraction, N2 adsorption, H2-N2O titration, temperature programmed reduction and scanning electron microscopy. X-ray diffraction characterizations revealed that Al^（3＋） can be doped in aurichalcite lattice, and the maximum doping amount of Al^（3＋） was 5.0% of total Cu and Zn atoms. The Cu/ZnO/Al2O3 sample produced by the modified method, in which co-precipitated Al^（3＋） was 2.5% of total Cu and Zn atoms showed much better activity and stability in water-gas shift reaction than commercial sample. The high Cu surface area（26.1 m^2/g） obtained by decompositon of doped aurichalcite is believed to be responsible for the activity enhancement. The stability was enhanced mainly because of the support effect of γ-Al2O3, which was decomposed from pseudo-boehmite in the calcination step.

关键词： Cu/ZnO/Al2O3 co-precipitation water-gas shift aurichalcite

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