摘要
Anatase TiO2 nanosheets(-ns-) with dominant exposed {001} facets were used as support to load copper,and the synthesized Cu/TiO2-ns catalysts were evaluated for CO2 hydrogenation to methanol. Under the reaction conditions, P = 3.0 MPa, T = 260 ℃, V(N2):V(H2):V(CO2) = 8:69:23 and gas hourly space velocity(GHSV) = 3600 mL g-1h-1, the methanol yield reached an appealing high value, 5.6%. Copper-loading amount, calcination temperature and reduction atmosphere have been investigated in this work, which significantly influence the particle sizes of copper and/or the defect concentration in TiO2, then leading to different catalytic performance. Characterizations of XRD, EPR, CO2-TPD and FTIR demonstrate that higher specific surface area of Cu is good for the hydrogenation of CO2 and adequate amount of Ti3+ plays important roles in CO2 activation. Both of them facilitate high turnover frequency(TOF) of methanol formation.
Anatase TiO2 nanosheets(-ns-) with dominant exposed {001} facets were used as support to load copper,and the synthesized Cu/TiO2-ns catalysts were evaluated for CO2 hydrogenation to methanol. Under the reaction conditions, P = 3.0 MPa, T = 260 ℃, V(N2):V(H2):V(CO2) = 8:69:23 and gas hourly space velocity(GHSV) = 3600 mL g-1h-1, the methanol yield reached an appealing high value, 5.6%. Copper-loading amount, calcination temperature and reduction atmosphere have been investigated in this work, which significantly influence the particle sizes of copper and/or the defect concentration in TiO2, then leading to different catalytic performance. Characterizations of XRD, EPR, CO2-TPD and FTIR demonstrate that higher specific surface area of Cu is good for the hydrogenation of CO2 and adequate amount of Ti3+ plays important roles in CO2 activation. Both of them facilitate high turnover frequency(TOF) of methanol formation.
基金
financially supported by the National Natural Science Foundation of China (no. 91645119, 21207039, B5151050)
the Fundamental Research Funds for the Central Universities (No.2017ZD076)
Guangzhou science and technology plan (201607010095)
the Natural Science Foundation of Guangdong Province, China (Grant no. S2011010000737)
State Key Laboratory of Physical Chemistry of Solid Surfaces, Xiamen University, P.R. China (No. 201602)