Deoxygenation reactions of nitrous oxide assisted by oriented external electric field

• Published in: International journal of quantum chemistry 2024-05, Vol.124 (9), p.n/a
• Main Authors: Zhang, Ming‐Xia, Li, Jun, Lei, Hao, Chen, Jia‐Hui, Sun, Peng‐Yang, Yao, Meng‐Ting, Liu, Lin, Guo, Jia
• Format: Article
• Language: English
• Subjects: Deoxygenation; deoxygenation reaction; Electric fields; Field strength; Greenhouse gases; Nitrous oxide; oriented external electric field; Solvent effect
• ISSN: 0020-7608; 1097-461X
• DOI: 10.1002/qua.27384

Due largely to the high stability and the potential ozone‐depleting, the transformation of greenhouse gas nitrous oxide has gained much attentions. In present paper, a new insight into the deoxygenation of nitrous oxide with silane was reported by using oriented external electric field (OEEF) as a catalytic strategy. When the OEEF was employed, the reaction barrier of deoxygenation was marvelously decreased as it was oriented along the positive NO/OSi bond‐axis. Especially the field strength is 300 × 10−4 a.u., the differences are up to 22.4/18.3 kcal mol−1 as compared with that of nonfield. In addition, once the H atom in SiH4 was replaced by methyl, two reaction modes were obtained, in which the deoxygenation process was easier when the N2O captured the H atom attached to the Si atom, not attached to the C atom. Further, the solvent effects of deoxygenation reaction were also considered, but with a weak influence were obtained. The deoxygenation reactions of greenhouse gas N2O were studied through a novel strategy—oriented external electric field (OEEF) based on DFT calculations. The results demonstrated that OEEF catalyzed this reaction obviously when it was oriented along the positive NO/OSi bond‐axis with the field strength added to 300 × 10−4 a.u.