【摘要】 二氧化碳（CO₂）通过加氢转化为乙醇等高附加值的化学品是实现“双碳”目标的重要途径之一。制备不同官能团（—OH和—NH₂）修饰的UiO-66负载Rh催化剂Rh/UiO-66,在间歇高压反应釜中评价所制备催化剂对CO₂加氢制乙醇反应的催化性能，并结合X射线衍射、扫描电子显微镜、透射电子显微镜等表征方法，探究官能团改性对Rh基催化剂上CO₂加氢反应性能的影响。结果表明：与Rh/UiO-66催化剂相比，经官能团修饰后催化剂的催化性能明显增强，尤其是经—NH₂修饰的催化剂（Rh/UiO-66-NH₂）表现出了优异的催化活性、乙醇选择性和循环稳定性；—NH₂修饰后，催化剂中Rh⁺含量明显增加，有利于稳定CO*,并促进其与CH_x*发生C—C偶联和加氢反应生成乙醇；在压力为3.0 MPa、温度为250℃的条件下，Rh/UiO-66-NH₂催化CO₂加氢反应的CO₂转化率为5.6%,乙醇选择性高达84.7%,且5次循环反应后催化剂性能基本不变。更多还原

【Abstract】 The hydrogenation of carbon dioxide（CO₂） to ethanol and other value-added chemicals is one of the important routes to achieve “dual-carbon” goals. Rh-based catalysts supported on UiO-66 modified with different functional groups（—OH and —NH₂） were prepared, their catalytic performance for CO₂ hydrogenation was tested in a batch reactor, and the effect of functional group modification on the performance of Rh-based catalysts for CO₂ hydrogenation was investigated by XRD,SEM,TEM,FT-IR,ICP,BET,TG,CO pulse, XPS and CO₂-TPD. The results showed that the catalytic performance of the catalyst modified with functional groups was significantly enhanced compared with that of Rh/UiO-66 catalyst. In particular, the Rh/UiO-66-NH₂ catalyst modified with —NH₂ exhibited excellent catalytic activity, ethanol selectivity and catalytic stability; while the Rh⁺ content in catalyst increased obviously after —NH₂ modification, which was beneficial to the stabilization of CO*,C—C coupling and hydrogenation with CH_x* were promoted to produce ethanol. At the pressure of 3.0 MPa and the temperature of 250 ℃,Rh/UiO-66-NH₂ exhibited the highest catalytic activity（5.6%） and ethanol selectivity（84.7%） with basically unchanged catalytic performance after five cycles.更多还原