题名V2O5/TiO2催化剂催化氧化氯代芳烃的机理研究
作者王健
学位类别硕士
答辩日期2013-05-01
授予单位中国科学院研究生院
导师朱廷玉 ; 王雪
关键词在工业烟气中 高氯代苯 当NH3-SCR反应与氯苯催化氧化共存时 (2)V2O5/TiO2催化剂催化氯苯的作用机理为:a氯苯发生亲核取代 b表面酚盐物种进一步氧化成邻苯二酚盐和对苯二酚盐物种 c苯二酚盐物种进一步氧化形成苯醌 d苯醌发生分解 (3)O2浓度提高有利于催化氧化反应的进行 向氯苯催化体系中引入NH3-SCR反应后 NH3与氯苯之间发生竞争吸附 氯苯 催化 SCR 机理 常见的氯代芳烃污染物有氯苯 多氯联苯和二恶英可归于持久性有机污染物(POPs) 探索了其影响氯苯催化反应的过程和机制。 本论文得出以下结论: (1)V2O5/TiO2催化剂对苯 在催化剂表面形成表面酚盐物种 即环状结构得到破坏形成马来酸 H2O的引入对催化反应有抑制作用 NO的存在对氯苯催化有促进作用 导致氯苯催化转化率下降。 本论文的研究工作为V2O5/TiO2催化剂在工业烟气催化降解氯代芳烃领域的应用提供了实验和理论依据。 关键词:V2O5/TiO2 氯酚 虽然含量低 苯酚 醋酸以及醛类物质 促进作用来源于NO与催化剂作用形成的表面NO2物种和硝酸盐物种 多氯联苯以及二恶英。其中 但毒性巨大 氯苯 并进一步氧化生成CO 但由于高温时催化剂表面硝酸盐物种减少使这种促进作用变得微弱 氯苯 严重危害人体健康 1 CO2 1 污染生态环境。 催化氧化法是去除工业烟气中氯代芳烃污染最为有效的方法之一。本文使用V2O5/TiO2催化剂 3-二氯苯和1 H2O和HCl最终完成氯苯的催化氧化过程 2二氯苯和1 针对苯 3 3-二氯苯符合挥发性有机化合物(VOCs)的定义 苯酚 5-三氯苯催化氧化机制是类似的 具有很强的挥发性 氯苯 Cl官能团数量增加 1 催化反应活性降低 3-二氯苯 1 3 5-三氯苯进行了活性评价和原位红外研究 提出了氯代芳烃催化降解过程中的具体步骤 并对苯环上不同官能团以及Cl官能团数量对于催化过程的具体影响进行了探索。另外 研究了烟气中复杂组分对氯苯催化氧化过程的影响
其他题名Mechanism study on catalytic oxidation of chlorinated aromatics over V2O5/TiO2 catalysts
学位专业环境工程
英文摘要In industrial flue gas, chlorobenzene, chlorophenols, PCBs and dioxins are the most common chlorinated aromatic pollutants, can be attributed to persistent organic pollutants (POPs). Chlorobenzene, 1,2-dichlorobenzene and 1,3-dichlorobenzene meet the definition of volatile organic compounds (VOCs), and are highly volatile; although the concentration of high-chlorinated benzene, PCBs and dioxins is low, they are very toxic, can cause serious harm to human health and ecological environment pollution. Catalytic oxidation method is an effective method to remove chlorinated aromatics from industrial flue gas. In this paper, Benzene, phenol, chlorobenzene, 1,3-dichlorobenzene and 1,3,5-trichlorobenzene were employed in catalytic experiments and in situ FTIR studies over V2O5/TiO2 catalyst. In particular, the impact of substituent group and the relative number of chlorine substituent on aromatic ring were studied, and a common catalytic mechanism was proposed. In addition, the impact of complex components in flue gas towards catalytic oxidation of chlorobenzene is investigated; when NH3-SCR reaction and chlorobenzene catalytic oxidation both exist in catalytic system, the effects of NO and NH3 regarding catalytic oxidation of chlorobenzene were presented. In this article, the following results are achieved: (1) A similar mechanism is operating during catalytic oxidation of benzene, phenol, chlorobenzene, 1,3-dichlorobenzene and 1,3,5-trichlorobenzene over V2O5/TiO2 catalyst; the catalytic activity of chlorinated benzene is reduced with increasing number of Cl substituent. (2) The main oxidation processes are as follows: 1) phenolates was obtained through a substitution process; 2) catecholates and quinolates were formed through phenolates; 3) further oxidation causing the formation of o- and p-benzoquinone-type species by catecholates and quinolates; 4) decomposition of benzoquinones and oxidation of non-aromatic compounds to form the final products. (3) The increasing of O2 concentration is beneficial towards catalytic oxidation of chlorobenzene, the introduction of H2O inhibit the catalytic reaction; when NH3-SCR reaction is introduced into catalytic system, catalytic oxidation of chlorobenzene can be promoted by surface NO2 species and nitrate species originated from adsorption of NO; competitive adsorption between NH3 and chlorobenzene can decline catalytic conversion rate of chlorobenzene. The research in this paper can provide a support for employing V2O5/TiO2 catalyst in the field of removing chlorinated aromatics from flue gas. Key words: V2O5/TiO2; Chlorobenzene; Catalytic; SCR; Mechanism
语种中文
公开日期2014-06-26
页码83
内容类型学位论文
源URL[http://ir.ipe.ac.cn/handle/122111/8367]  
专题过程工程研究所_研究所(批量导入)
推荐引用方式
GB/T 7714
王健. V2O5/TiO2催化剂催化氧化氯代芳烃的机理研究[D]. 中国科学院研究生院. 2013.
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