碳基材料纳孔空间内SO2吸附转化机理  

Mechanism of SO2 Adsorption and Conversion in Nanopores of Carbon-based Materials

作　　者：孙飞[1] 高继慧[1] 曲智斌 刘欣[1] 皮信信 郄志鹏[1] SUN Fei;GAO Jihui;QU Zhibin;LIU Xin;PI Xinxin;QIE Zhipeng(School of Energy Science and Engineering Harbin Institute of Technology,Harbin 150001,Heilongjiang Province,China)

机构地区：[1]能源科学与工程学院(哈尔滨工业大学)

出　　处：《中国电机工程学报》2019年第20期5979-5988,共10页Proceedings of the CSEE

基　　金：国家重点研发计划项目(2017YFB0602901)~~

摘　　要：活性焦脱硫过程中SO2在纳孔内发生吸附、转化、迁移,这些过程受孔结构和表面化学性质的共同影响。揭示碳材料纳孔内SO2吸附转化机理是发展SO2资源化脱除技术的理论基础。综述团队围绕碳材料纳孔内SO2吸附转化机理开展的研究:1)利用典型活性焦材料,揭示纳孔中SO2在O2和H2O作用下的吸附转化机理;2)通过量子化学计算明确碳材料内催化氧化SO2的活性位;3)揭示微孔、中大孔在SO2吸附、转化、迁移中的作用,指出理想的脱硫碳材料应具有的孔隙结构;4)基于分子自组装技术制备模型碳材料,单因素研究了含氮官能团对SO2吸附转化影响。研究揭示碳材料纳孔内SO2吸附转化机理,为SO2资源化脱除技术的发展提供了理论参考。The desulfurization by activated coke contains multiple steps such as SO2 adsorption, conversion and H2 SO4 migration in nanopores and is influenced by pore structures and surface chemistry simultaneously. Revealing the mechanism of SO2 adsorption and conversion in carbon-based nanopores are the theoretical bases for resource utilization of SO2. We reviewed our researches on the mechanism of SO2 adsorption and conversion in nanopores of carbon-based materials: 1) By using typical activated coke for SO2 removal kinetic experiments, the adsorption and conversion mechanism of SO2 in carbon-based nanopores in the presence of O2 and H2 O was revealed;2) The active sites for SO2 catalytic oxidation and the role of H2 O were demonstrated via quantum chemistry calculations;3) The role of mesopores and macropores in SO2 adsorption, conversion and transfer was revealed and the ideal pore structures for SO2 was proposed;4) To reveal the role of so-called active sites in SO2 adsorption and conversion, the effect of nitrogen-containing functional groups on SO2 adsorption was independently determined by preparing a series of model carbon materials with gradient nitrogen content and consistent pore structure via molecular self-assembly. Above researches systematically reveal the mechanism of SO2 adsorption and conversion in carbon-based nanopores, and provide theoretical guidance for the development of advanced SO2 resource utilization technology.

关 键 词：碳材料 纳孔空间 SO2 资源化 极性致迁移 

分 类 号：TK9[动力工程及工程热物理]