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V2O5/TiO2催化剂催化氧化氯代芳烃的机理研究
Alternative TitleMechanism study on catalytic oxidation of chlorinated aromatics over V2O5/TiO2 catalysts
王健
Subtype硕士
Thesis Advisor朱廷玉 ; 王雪
2013-05-01
Degree Grantor中国科学院研究生院
Degree Discipline环境工程
Keyword在工业烟气中 常见的氯代芳烃污染物有氯苯、氯酚、多氯联苯以及二恶英。其中 高氯代苯、多氯联苯和二恶英可归于持久性有机污染物(pops) 氯苯、1 虽然含量低 当nh3-scr反应与氯苯催化氧化共存时 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 2二氯苯和1 但毒性巨大 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、苯酚、氯苯、1 (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 C苯二酚盐物种进一步氧化形成苯醌 3-二氯苯符合挥发性有机化合物(vocs)的定义 严重危害人体健康 3-二氯苯和1 在催化剂表面形成表面酚盐物种 具有很强的挥发性 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 针对苯、苯酚、氯苯、1 5-三氯苯催化氧化机制是类似的 D苯醌发生分解 3-二氯苯、1 Cl官能团数量增加 即环状结构得到破坏形成马来酸、醋酸以及醛类物质 (3)o2浓度提高有利于催化氧化反应的进行 3 催化反应活性降低 并进一步氧化生成co、co2、h2o和hcl最终完成氯苯的催化氧化过程 H2o的引入对催化反应有抑制作用 向氯苯催化体系中引入nh3-scr反应后 氯苯 Nh3与氯苯之间发生竞争吸附 5-三氯苯进行了活性评价和原位红外研究 No的存在对氯苯催化有促进作用 催化 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 提出了氯代芳烃催化降解过程中的具体步骤 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 Scr 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 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 机理 研究了烟气中复杂组分对氯苯催化氧化过程的影响
Other AbstractIn 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
Pages83
Language中文
Document Type学位论文
Identifierhttp://ir.ipe.ac.cn/handle/122111/8367
Collection研究所(批量导入)
Recommended Citation
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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