Comparative insight into activation of methane by ScAl2O2− and Sc from a theoretical study

• Published in: Computational and theoretical chemistry 2023-10, Vol.1228, p.114237, Article 114237
• Main Authors: Junxi, Liang, Bomiao, Qi, Yu, Duan, Mengmeng, Lu, Fupeng, Zhang, Weimin, Jia, Shaofeng, Pang, Yanbin, Wang, Qiong, Su
• Format: Article
• Language: English
• Subjects: CH4 activation; Density functional calculation; Mechanism; ScAl2O2
• ISSN: 2210-271X
• DOI: 10.1016/j.comptc.2023.114237

The Sc atom is particularly significant role in the ScAl2O2− activating methane CH bond, so the creation of H2 suggests that the importance of the “support” cluster cannot be overlooked. In the reaction of CH activated by Sc atom, the energy of the single state is lower than that of the triplet state. There is an orbital drill-through effect, in which the single state is the major channel of the reaction. ScAl2O2− catalyzes the activation of CH4 to get the H2, which serves as a candidate for the production of new energy. [Display omitted] Due to its thermochemical stability, CH4 is generally difficult to be dissociated. In this paper, the role of Sc atom in the results of the CH bond activation operation was investigated using the DFT-D (M06-2X) method to understand the reaction process. It was discovered that the double low-spin state Sc atom easily react with CH4, whereas the high-spin ground state Sc is inert. The mechanism of the supported ScAl2O2− activated CH4 and the free Sc reaction system are extremely similar. The major channel is the low-spin state, displaying the incidence of spin flipping has an orbital drill-through effect. In the ScAl2O2− reaction, the Al2O2− anion can efficiently support Sc atom and thereby activate CH4 while also imparting its high reactivity to the supported Sc. In the future, it will be possible to examine the role of the Sc atom in the catalytic activation process of ScAl2O3− on CH4.