【摘要】 采用表面反应改性法制备了ZrO2 SiO2 (ZrSiO)表面复合物 ,用等体积浸渍法制备了ZrSiO担载的Cu Ni双金属催化剂 ,并用IR ,TPD ,TPSR和微反技术考察了CO2 和CH3 OH在催化剂表面上的化学吸附及反应性能 .实验结果表明 :在Cu Ni/ZrSiO催化剂上存在着Cu Ni金属位M ,Lewis酸位Zrn + 和Lewis碱位Zr O-三类活性中心 ;CO2 在金属位和Lewis酸位的协同作用下可形成CO2 卧式吸附态 ,此吸附态在 142℃左右可解离成M CO和Zr O-;CH3 OH在Lewis酸位和Lewis碱位的协同作用下可形成解离吸附态Zr OCH3 和Zr OH ;CO2 和CH3 OH在Cu Ni/ZrSiO催化剂表面上的主要反应产物为碳酸二甲酯 (选择性在 85 %以上 ) ,另有少量的CH2 O ,CO和H2 O .更多还原

【Abstract】 The surface complex support ZrO 2 SiO 2 (ZrSiO) was prepared by surface reaction modification, and Cu Ni/ZrSiO bimetallic catalyst was prepared by isovolumic impregnation. Adsorption and reaction of CO 2 with CH 3OH on the catalyst were characterized by IR, TPD, TPSR and microreactor techniques. The results showed that there exist three kinds of active sites on the catalyst: metal site M, Lewis acid site Zr n + and Lewis basic site Zr O -; CO 2 horizontal adsorption state, formed from its shearing state on M with the cooperation of adjacent Zr n + , can be dissociated into M CO and Zr O - at about 142 ℃ and CH 3OH dissociated into Zr OCH 3 and Zr OH with the cooperaton of Zr n + and adjacent Zr O -; the main reaction products on the catalyst are dimethyl carbonate (DMC) with a selectivity of over 85%, and less amounts of CH 2O, CO and H 2O.更多还原