炭材料空位、氮掺杂和受限空间协同催化氧化SO2机理研究

项目名称： 炭材料空位、氮掺杂和受限空间协同催化氧化SO2机理研究

项目编号： No.51508356

项目类型： 青年科学基金项目

立项/批准年度： 2016

项目学科： 其他

项目作者： 岑望来

作者单位： 四川大学

项目金额： 20万元

中文摘要： 多孔炭基催化剂能在100℃以下直接利用烟气中的H2O、O2和SO2生成硫酸，与工业制硫酸高达400℃的反应温度形成对比，这一奇特现象至今没有得到明确的机理性解释。申请者在前期探索中发现，单个SO2和H2SO3分子极易被炭材料表面活性氧物种氧化，本申请拟在此基础上，针对炭材料中孔隙结构内的催化脱硫反应和氮掺杂促进脱硫性能现象中的关键科学问题，采用分子动力学和第一性原理相结合的计算模拟方法，系统研究孔道受限空间与孔内碳原子空位对H2O/O2/SO2混合体系的吸附、扩散、氧化和产物硫酸脱附的影响规律，据此阐明空位与炭材料受限空间协同催化氧化SO2机理。运用计算模拟与化学气相沉积和原位红外实验相结合的研究方法，研究氮掺杂类型和含量对反应物吸附和反应特性的影响规律，明确氮掺杂促进催化脱硫的原理，为脱硫炭材料的氮掺杂改性提供理论指导。

中文关键词： 烟气脱硫；碳纳米管；氮掺杂；计算模拟；石墨烯

英文摘要： Compared to the industrial production of sulfuric acid at a temperature as high as 400℃，the SO2 of flue gases can be straightforward catalytically oxidized to form sulfuric acid by porous carbon-based catalyst in the presence of O2 and H2O. No clear mechanism has been proposed yet for the unique process. In our recent explorations, isolated SO2 and H2SO3 molecules were found to be oxidized with rather low barriers. On the basis of these tasks, aimed to uncover the key scientific problems on the catalytic desulfurization processes in pores of carbon materials and the promotion effects of N-doping, the first-principles and molecular dynamic methods will be used combined to investigate the adsorption, diffusion, reaction and sulfuric acid desorption in the confined pore spaces systematically. The effects of carbon vacancies on the wall will be investigated as well. A synergetic mechanism for the catalytic oxidation of SO2 between vacancies and confined space will be proposed subsequently. Computational simulation and experimental methods will be used combined to investigate the adsorption and reaction in the pores of carbon materials due to the N-doping pattern and content. The experimental methods include chemical vapor deposition and in situ infrared spectroscopy. The promotion mechanism by N-doping will be clarified, which provide theoretical guidance for the N-doping fabrication of carbon catalyst.

英文关键词： flue gas desulfurization;carbon nanotube;Nitrogen doping;computational simulation;graphene