课题组近期研究发现,通过制备方法能实现CoCe复合催化剂孔结构调控,并调控其CO2催化加氢性能。通过XRD、BET、TEM/HTEM和H2-TPD对制备的催化剂的物理化学性质进行了表征。表征结果表明,合适的制备方法能促进Co物种溶入CeO2晶格形成Ce-O-Co固溶体,这可促进相应的Co物种被H2还原形成活性Co0物种。硬模板法制备的CoCe-HT催化剂前驱体具有大的比表面积和发达有序的介孔结构,这有利于活性Co0物种形成,从而促进H2活化形成活性H物种。所研究的CoCe复合催化剂的CO2加氢活性遵从如下顺序:CoCe-HT > CoCe-CP > CoCe-CA > CoCe-HY。CoCe-HT催化剂展现高的CO2加氢转化率,在360 °C时可达53.9%,且在600 min内能保持良好的稳定性。然而,通过络合法制得的CoCe-CA催化剂具有较差的使用稳定性。
Guilin Zhou* (周桂林), Liying Xie, Fengqiong Xie, Shuang Chen, Jia Zeng, Hongmei Xie. CoCe composite catalyst for CO2 hydrogenation: Effect of pore structure [J]. Journal of the Energy Institute, 2024, 117: 101856.
https://doi.org/10.1016/j.joei.2024.101856
In order to realize the dual carbon goals of “carbon peaking” and “carbon neutrality”, the design and development CO2 hydrogenation catalyst with high performances is of great significance. In this study, the CoCe composite catalysts were prepared by different methods and used to CO2 catalytic hydrogenation. The physicochemical properties of the prepared catalysts were characterized by XRD, BET, TEM/HRTEM, and H2-TPD. The characterization results indicated that the studied CoCe composite catalysts with different pore structure can be prepared by different preparation methods. The suitable preparation method can promote Co species to be dissolved into the CeO2 lattice to form Ce-O-Co solid solution, which can promote the corresponding Co species to be reduced by H2 to form active Co0 species. The large specific surface area and developed ordered mesoporous structure of the CoCe-HT catalyst precursor, which was prepared by hard-template method, are conducive to the formation of active Co0 species and activation of H2 to produce reactive H species. The CO2 hydrogenation activity of the studied CoCe composite catalysts follows the following order: CoCe-HT > CoCe-CP > CoCe-CA > CoCe-HY. The CoCe-HT catalyst showed high CO2 hydrogenation conversion of 53.9% and good using stability at 360 °C for 600 min. However, the CoCe-CA prepared by complex method has a poor use stability.