Si-CNT循环催化N2O与CO反应的理论研究

Theoretical investigation for the reaction of N2O and CO catalyzed by Si-CNT

通过非金属催化转化有毒气体来解决环境问题已经成为最有效最有前景的方法.基于密度泛函理论(Density Functional Theory,DFT)研究了Si掺杂碳纳米管(Si-CNT)催化氧化N2O与CO的反应.N2O分子更易以直线形式吸附在Si-CNT催化剂上,并分解为N2和CNT-SiO中间体,对应的活化能垒为2.42 kJ/mol.CNT-SiO中间体很活泼很容易与CO继续反应生成CO2.通过分析发现CNT既可以作为电子的接受体又可以作为电子的供体,因此帮助了电荷在Si和目标分子之间的转移,这将为探索其它类似催化剂起到一定的帮助作用.

Non-metal catalysis of harmful gases maybe the most promising and important way for solving environmental problems.We applied a density functional theory(DFT)to investigate the CO oxidation by using N2O as an oxidizing agent over a Si-embedded carbon nanotube(Si-CNT)catalyst.The N2O molecule is more likely to adsorb on the Si-CNT by linear structure,and yield to N2 and CNT-SiO intermediate with the activation energy of 2.42 kJ/mol.CNT-SiO is an active intermediate which is easy to react with the CO to form CO2.According to the analysis,the CNT acts as both the electron withdrawing and donating support to assist the charge transfer between the Si atom and the probe molecules.This may open new avenues in searching for oxidation of CO at an economical cost.