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Catalytic hydrogenation of CO2 to aromatics over indium-zirconium solid solution and sheet HZSM-5 tandem catalysts
Applied Surface Science ( IF 6.3 ) Pub Date : 2024-09-02 , DOI: 10.1016/j.apsusc.2024.161155
Haifeng Tian , Chunxue Jiao , Qingchao Li , Zhiyu Chen , Haowei Huang , Fei Zha , Xiaojun Guo , Xiaohua Tang , Hongshan Chen

The presence of acids and bases, coupled with its exceptional CO adsorption capacity and thermal stability, has established zirconia as a highly esteemed promoter and carrier. Researchers have found that the InO supported ZrO exhibits high activity and remarkable stability. Therefore, xIn-yZr(T) solid solutions were prepared with different calcination temperatures and In/Zr molar ratios. The solid solutions were then combined with sheet HZSM-5 zeolite from tandem catalysts, which were investigated for their catalytic performance in converting CO to aromatics. The X-ray diffraction, scanning electron microscopy, N adsorption-desorption, NH temperature-programmed desorption, pyridine infrared radiation, X-ray photoelectron spectroscopy, electron paramagnetic resonance, CO temperature-programmed desorption and H temperature-programmed reduction characterization methods were used to investigate the physicochemical properties of catalysts. Density Functional Theory calculations were used to investigate the energy of thermal desorption and H reduction to generate oxygen vacancies on the surface of InO(111) and Zr/InO(111). Additionally, the influence of oxygen vacancies on CO adsorption energies was simulated. It was found that the incorporation of a moderate amount of zirconium carriers promoted the generation of oxygen vacancies and provided better metal-carrier interactions. The 4In-1Zr(500 °C)/HZSM-5 tandem catalyst exhibits excellent catalytic stability, achieving a CO conversion of 24.3 % and aromatics selectivity of 37.3 %.

中文翻译:


铟锆固溶体和片状HZSM-5串联催化剂催化CO2加氢制芳烃



酸和碱的存在,加上其卓越的 CO 吸附能力和热稳定性,使氧化锆成为备受推崇的促进剂和载体。研究人员发现,In2O3负载的ZrO表现出高活性和显着的稳定性。因此,采用不同的煅烧温度和In/Zr摩尔比制备了xIn-yZr(T)固溶体。然后将固溶体与串联催化剂中的片状 HZSM-5 沸石结合,研究其将 CO 转化为芳烃的催化性能。采用X射线衍射、扫描电镜、N2吸附-脱附、NH3程序升温脱附、吡啶红外辐射、X射线光电子能谱、电子顺磁共振、CO程序升温脱附和H2程序升温还原表征方法研究催化剂的物理化学性质。采用密度泛函理论计算研究了热脱附和H还原在InO(111)和Zr/InO(111)表面产生氧空位的能量。此外,还模拟了氧空位对CO吸附能的影响。研究发现,加入适量的锆载体可以促进氧空位的产生,并提供更好的金属-载体相互作用。 4In-1Zr(500 °C)/HZSM-5串联催化剂表现出优异的催化稳定性,实现了24.3%的CO转化率和37.3%的芳烃选择性。
更新日期:2024-09-02
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