为构筑用于高效活化CO₂并兼具较高低碳烯烃选择性的双功能催化剂,采用MOF膜控沸石核壳复合催化剂的组装策略制备了ZnZrGaO_x/SAPO-34@UiO-66双功能催化剂,并将其用于催化CO₂加氢。探究了不同摩尔比ZnZrGaO_x与SAPO-34及SAPO-34@UiO-66的协同作用。结果表明,ZnZrGaO_x/SAPO-34对于低碳烯烃(C⁼₂~C⁼₄)的选择性只有62.38%,而ZnZrGaO_x/SAPO-34@UiO-66对C⁼₂~C⁼₄的选择性达到81.57%。证明UiO-66在SAPO-34的表面均匀包覆能调节沸石的酸性及表面笼数量,进而影响产物的分布,促进烷烃向烯烃转变。

In order to construct a bifunctional catalyst for efficiently activating CO₂ with relatively high selectivity for low-carbon olefins,an assembly strategy of MOF membrane-controlled zeolite core-shell composite catalysts is employed to prepare ZnZrGaO_x/SAPO-34@UiO-66 bifunctional catalyst that is applied in the catalytic hydrogenation of CO₂.The synergy between different molar ratios of ZnZrGaO_x to SAPO-34 and SAPO-34@UiO-66 is investigated.It is found that the selectivity of ZnZrGaO_x/SAPO-34 for C⁼₂-C⁼₄ is merely 62.38%,while that of ZnZrGaO_x/SAPO-34@UiO-66 reaches 81.57%.It is demonstrated that the uniform coating of UiO-66 on the surface of SAPO-34 can regulate the acidity of the zeolite and the number of surface cages,thereby influencing the distribution of products and facilitating the transformation from alkanes to olefins.

赵爱勤(1995),女,硕士生,研究方向为CO₂加氢制低碳烯烃双功能催化剂的制备及性能研究,15649853023@163.com;许海涛(1969),男,博士,副教授,研究方向为微介孔材料的制备及CO₂催化转化,通讯联系人,xuhaitao@ecust.edu.cn。