Tao Miao, Zhou Changlu, Shi Yaoqi, Meng Xin, Gu Jia, Gao Wenli, Xin Zhong
Shanghai Key Laboratory of Multiphase Materials Chemical Engineering, East China University of Science and Technology People's Republic of China
State Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology Shanghai People's Republic of China.
RSC Adv. 2020 Jun 2;10(35):20852-20861. doi: 10.1039/d0ra02168g. eCollection 2020 May 27.
According to its thermodynamic equilibrium analysis and strong exothermic characteristics, the major challenge of syngas methanation is to develop a high-efficient low-temperature catalyst with superior sintering resistance. In this study, bimetal-based SBA-15 catalysts were prepared a citric acid-assisted impregnation method and applied in CO methanation. The obtained catalysts were characterized X-ray diffraction, N adsorption-desorption, high-resolution transmission electron microscopy, X-ray photoelectron spectroscopy, H temperature-programmed reduction and other techniques. Combining the structural characterization of the fresh and used catalyst, the function of the organic additive and metal promoters was revealed. The catalysts exhibited superior low-temperature activity and excellent sintering resistance owing to the electron migration from the additive metal to Ni, strong interaction between the metal and support and the confinement effect of the support. The catalyst with Mo as a promotor exhibited the best dispersion and the largest surface concentration of nickel, which resulted in its highest catalytic activity among the catalysts. The design and preparation of a highly effective catalyst can provide novel insight into the preparation of other catalysts.
根据其热力学平衡分析和强放热特性，合成气甲烷化的主要挑战是开发一种具有优异抗烧结性能的高效低温催化剂。在本研究中，采用柠檬酸辅助浸渍法制备了双金属基SBA-15催化剂，并将其应用于CO甲烷化反应。通过X射线衍射、N吸附-脱附、高分辨率透射电子显微镜、X射线光电子能谱、H程序升温还原等技术对所得催化剂进行了表征。结合新鲜催化剂和使用后催化剂的结构表征，揭示了有机添加剂和金属助剂的作用。由于添加剂金属向Ni的电子迁移、金属与载体之间的强相互作用以及载体的限域效应，催化剂表现出优异的低温活性和抗烧结性能。以Mo为助剂的催化剂表现出最佳的分散性和最大的镍表面浓度，这导致其在催化剂中具有最高的催化活性。高效催化剂的设计和制备可为其他催化剂的制备提供新的思路。
