Experimental and theoretical study of the intrinsic kinetics for dimethyl ether synthesis from CO2 over Cu–Fe–Zr/HZSM-5
Experimental and theoretical study of the intrinsic kinetics for dimethyl ether synthesis from CO2 over Cu–Fe–Zr/HZSM-5
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DOI：
10.1002/aic.14743
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发表时间：
2015-05
期刊：
影响因子：
3.7
通讯作者：
Zuzeng Qin;Tongming Su;Hongbing Ji;Yuexiu Jiang;Li Ruiwen;Jian-hua Chen
中科院分区：
文献类型：
--
作者：
Zuzeng Qin;Tongming Su;Hongbing Ji;Yuexiu Jiang;Li Ruiwen;Jian-hua Chen
An intrinsic kinetics model was established for CO2 hydrogenation to dimethyl ether (DME) with a Cu–Fe–Zr/HZSM-5 catalyst based on H2/CO2 adsorption, simulation, and calculation of methanol synthesis from CO2 intermediates and experimental data. H2/CO2-temperature programmed desorption results show a dissociative H2 adsorption on Cu site; CO2 was linearly adsorbed on Fe3O4 weak base sites of the catalyst; the adsorbing capacity of H2 and CO2 increased after Zr-doping. Density functional theory analysis of methanol synthesis from CO2 and H2 revealed a formate pathway. Methanol synthesis was the rate-limiting step (173.72 kJ·mol−1 activation energy) of the overall CO2 hydrogenation reaction, and formation of H2CO is the rate-determining step of methanol synthesis. Relative errors between calculated and experimental data of partial pressures of all components were less than 10%. Therefore, the kinetics model may be an accurate descriptor of intrinsic kinetics of CO2 hydrogenation to DME. © 2015 American Institute of Chemical Engineers AIChE J, 61: 1613–1627, 2015
