CO_(2)加氢合成甲醇MO_(x)/In_(2)O_(3)(M=Zn,Ga,Zr)催化剂的研究

Hydrogenation of CO_(2) to Methanol over MO_(x)/In_(2)O_(3)(M=Zn,Ga,Zr)Catalyst

氧化铟作为单一金属氧化物,可催化CO_(2)分子高选择性加氢合成甲醇。为进一步提升其催化性能,采用氧化物之间的相互作用对氧化铟催化剂掺杂改性的策略,使用初湿浸渍法制备了MO_(x)/In_(2)O_(3)(M=Zn,Ga,Zr)催化剂。通过热重分析、X射线衍射和高分辨率透射电子显微镜对催化剂的结构和稳定性进行了讨论。实验结果表明,反应温度对催化活性有显著影响。所有催化剂的CO_(2)转化率随反应温度的升高而增加。特别地,甲醇的生成速率首先随反应温度的升高而增加,但当温度升高到330℃以上时开始降低。10%ZrO_(2)/In_(2)O_(3)催化剂的甲醇生成速率在330℃、3 MPa的反应条件下达到4.62 mol·h^(-1)·kg^(-1),明显优于氧化铟催化剂。最后讨论了ZrO_(2)的加入对催化反应的增强作用。

Indium oxide,as a single metal oxide,could catalyze the highly selective hydrogenation of CO_(2) molecules to synthesize methanol.In order to further improve its catalytic performance,a strategy of doping and modifying the indium oxide catalyst based on the interaction between oxides was adopted,and the MO_(x)/In_(2)O_(3)(M=Zn,Ga,Zr)catalyst was prepared using the incipient wetness impregnation method.The experimental results indicated that the reaction temperature had a significant effect on catalytic activi-ty.The structure and stability of the catalyst were discussed through thermogravimetric analysis,X-ray diffraction,and high-resolution transmission electron microscopy.The CO_(2) conversion rates of all cata-lysts increased with the increase reaction temperature.In particular,the methanol production rate first in-creased with the increase of reaction temperature,and it began to decrease when the temperature was a-bove 330℃.The highest methanol formation rate on the 10%ZrO_(2)/In2O_(3) catalyst was achieved at 330℃ and 3 MPa,at 4.62 mol·h^(-1)·kg^(-1),which was significantly superior to pure indium oxide.The promotion of ZrO_(2) on the catalytic reaction was also explored.