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课题组与重庆大学合作研究Co和Mn物种在CO2加氢反应中的协同效应取得进展
发布时间:2024-04-07

课题组近期研究发现,MnOx为催化剂载体,采用浸渍法制得的纳米xCo/MnO 催化剂对CO2加氢反应有良好的催化作用。xCo/MnO催化剂表面的中等碱性位是主要的CO2吸附位,而MnOx载体表面具有的大量中等碱性位,可增强xCo/MnO催化剂对CO2分子的吸附能力。通过改变Co物种在催化剂表面的负载量,可实现对xCo/MnO催化剂表面碱性位和加氢活性位数量的有效调控,进而改善xCo/MnO催化剂对CO2分子的吸附、活化和加氢性能。此外,发现在制备的xCo/MnO催化剂中形成了Mn1-yCoyO 固溶体,有利于促进金属Co纳米颗粒在MnO表面的分散和xCo/MnO催化剂表面氧缺陷位的生成。12Co/MnO催化剂上的CO2吸附量达到了1.76 mmol/g,使催化剂具有优越的CO2吸附和活化能力,并使其具有良好的CO2加氢性能。在常压和420 °C条件下,所制12Co/MnO催化剂的CO2转化率和CH4选择性分别达到了57.5%78.8%。在12Co/MnO催化剂上进行的10CO2加氢循环测试中,CO2转化率也始终保持在最初的57.5%CH4选择性保持在70.0%以上。


 Sheng Miao (苗盛), Shuang Chen, Jia Zeng, Zhenqiong Gou, Chuan Huang*, Xiang Wang, Guilin Zhou*. Synergistic effects between Mn and Co species in CO2 hydrogenation over xCo/MnO catalysts [J]. Fuel, 2024, 362: 130853.

https://doi.org/10.1016/j.fuel.2023.130853


      In this paper, the xCo/MnO catalysts for CO2 hydrogenation reaction were prepared by the impregnation method using MnOx as the catalyst support. The effects of the Co loading on the CO2 hydrogenation performances of the prepared xCo/MnO catalysts were investigated. The active Co0 species on the xCo/MnO catalysts surface are the main active centers for the CO2 hydrogenation reaction, and the medium basic sites on the xCo/MnO catalysts are the main CO2 adsorption sites. The MnOx support possesses a large number of medium basic sites, which enhance the CO2 molecules adsorption ability of the xCo/MnO catalysts. An effective regulation of the basic and hydrogenation active site numbers on the xCo/MnO catalysts surface can be achieved by changing the Co loading amount, which in turn can affect the CO2 molecules adsorption, activation and hydrogenation abilities of the xCo/MnO catalysts. Moreover, the Mn1-yCoyO solid solution was found to be formed in the prepared xCo/MnO catalysts, which is conducive to the dispersion of metal Co nanoparticles on the MnO surface and the generation of oxygen-deficient sites. The CO2 desorption amount on the 12Co/MnO catalyst reached 1.76 mmol/g, which provided the catalyst with strong CO2 adsorption and activation abilities, enabling it to exhibit great CO2 hydrogenation performance. Under the conditions of atmosphere and 420 ℃, the CO2 conversion and CH4 selectivity on the prepared 12Co/MnO catalyst reached 57.5% and 78.8%, separately. Furthermore, the CO2 conversion was able to consistently remain at the initial 57.5%, and the CH4 selectivity was maintained above 70% in the 10 times CO2 hydrogenation cycle tests on the 12Co/MnO catalyst.