课题组近期研究发现,类水滑石CoAlx-LDH前驱体的层状结构促进CoAlx-LD催化剂中高分散度的Co0活性中心的形成,有利于对反应物分子CH4和CO2的吸附和活化,促进了活性CHx(x < 4)和CO2δ-物种形成,可进一步促进DRM反应的进行。同时,Co物种与Al物种的协同作用能有效提升CoAl复合催化剂的催化性能。通过Co/Al摩尔比可有效调控CoAlx-LD催化剂表面Co0活性位、碱性位和氧空位数量,从而调控催化剂的CH4/CO2重整催化性能。Co/Al摩尔比为1/2的CoAl12-LD催化剂表现出优异的CH4/CO2重整催化性能。在常压和700 °C条件下,所制备的CoAl12-LD催化剂的CH4和CO2转化率分别达到86.8%和53.4%。此外,该催化剂在CH4/CO2重整反应也中表现出优异的使用稳定性。
Na Liu(刘娜), Hongmei Xie, Shuang Chen, Jia Zeng, Aiping Jia**, Guilin Zhou*. CoAl composite catalysts derived from hydrotalcite-like compounds for CH4 efficient dry reforming[J].International Journal of Hydrogen Energy 87 (2024) 1023-1034.
https://doi.org/10.1016/j.ijhydene.2024.09.078
In this study, CoAlx-LDHhydrotalcite-likewas used as the precursors to preparethe CoAlx-LD composite catalysts for the DRMreaction. The transition metal Co was the main catalytic active centers for the DRM reaction. The layered structure of the hydrotalcite-like CoAlx-LDH precursors promoted thehighly dispersed Co0 active centers to be formed in the CoAlx-LD catalysts. In addition, synergistic effects between active sites, basic sites and oxygen vacancies can promote the DRMcatalytic performances of CoAl composite catalysts. Meanwhile, the Co/Al mole ratio can regulate the active sites, basic sites and oxygen vacancies in the catalysts, thereby affecting its catalytic performances. The CoAl12-LD catalyst with a Co/Al mole ratio of 1/2 exhibited excellent DRM catalytic performances.TheCH4 and CO2 conversions on the prepared CoAl12-LD catalyst achieved 86.8% and 53.4% at atmospheric pressure and 700 °C, respectively. In addition, the catalyst alsoshowed excellent use stability in the DRM reaction.