期刊
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
卷 60, 期 36, 页码 13214-13222出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.iecr.1c02150
关键词
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资金
- Natural Science Foundation of Shanxi Province [201801D121056]
- Key Research and Development Project of Shanxi Province [201803D421011]
- National Natural Science Foundation of China [U1510203]
By adjusting the Cr:Mn:Ga atomic ratio to 3:2:1, a high CO conversion with light olefin selectivity was achieved under the appropriate reaction conditions, and increasing the Cr/Mn ratio facilitated the reduction of the CrMnGa catalyst and increased surface oxygen vacancies.
Metal oxide in a bifunctional catalyst plays crucial roles in catalytic activity for syngas conversion to olefin (STO). Here, ternary co-precipitated CrMnGa oxides with various Cr/Mn ratios were prepared and combined with SAPO-34 for an STO reaction. By adjusting the Cr:Mn:Ga atomic ratio to 3:2:1, a high CO conversion (43.5%) with light olefin selectivity (87.0%, CO2 free) is achieved under the reaction conditions of 400 degrees C, 3.0 MPa, and 3000 mL center dot h(-1)center dot g(-1). The increase in the Cr/Mn ratio facilitated the CrMnGa catalyst reduction and enhanced surface oxygen vacancies contents and H-2 dissociation ability. The mechanism reveals that *CH3O species act as the reaction intermediate for the reaction of CO with the surface OH group and the subsequent hydrogenation. More importantly, the introduction of Cr enhanced the CO activation ability at high temperatures and thus provided a well temperature match for intermediate generation over CrMnGa oxide and further transformation into light olefin over SAPO-34. This study provides a strategy for rational design of highly active metal oxides, which could be used to combine with other zeolites for syngas conversion to high value-added chemicals.
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