甲酸辅助Cu-ZnO-Al2O3催化剂制备及其CO2加氢制甲醇性能研究

Formic acid assisted synthesis of Cu-ZnO-Al2O3 catalyst and its performance in CO2 hydrogenation to methanol

    摘要
  • 摘要: 采用共沉淀法制备Cu/Zn/Al前驱体，经甲酸处理后N2气氛焙烧得到Cu-ZnO-Al2O3催化剂(CZA)用于CO2加氢制甲醇反应。使用XRD、BET、TG-DSC、SEM、H2-TPR、N2O滴定、XPS-AES、CO2-TPD表征技术对催化剂的物相组成、结构性质以及Cu物种的比表面积、分散度以及价态分布进行分析和讨论。结果表明，甲酸处理调节了催化剂中Cu+与Cu0的比例，同时增加催化剂的中强碱性，并提高甲醇选择性。在W/F(H2/CO2=70/23) = 10 g∙h/mol、t = 200 ℃、p = 3 MPa反应条件下，使用HCOOH/Cu（物质的量比）= 0.8甲酸处理获得的催化剂，CO2转化率6.7%，甲醇选择性达76.3%。

     

    Abstract: The Cu/Zn/Al precursor by coprecipitation was treated with formic acid and then calcined in N2 to obtain Cu-ZnO-Al2O3 catalyst (CZA) for the CO2 hydrogenation to methanol. XRD, BET, TG-DSC, SEM, H2-TPR, N2O titration, XPS-AES and CO2-TPD characterization techniques were used to analyze the phase composition, structural properties of the catalyst, the Cu specific surface area, the dispersion and valence of the Cu species. The results showed that the formic acid treatment tuned the ratio of Cu+ and Cu0, increased the number of medium-strong base sites in the catalyst, and raised the selectivity of methanol. Under reaction conditions of W/F(H2/CO2=70/23)=10 g∙h/mol, t =200 ℃ and p =3 MPa, using Cu-ZnO-Al2O3 treated under HCOOH/Cu (molar ratio) =0.8, the CO2 conversion and the methanol selectivity were 6.7% and 76.3%, respectively.

     

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