CAJ | 학술논문

活性炭表面物化性质是炭基催化剂催化TeCA脱HCl合成TCE反应性能的重要影响因素。采用酸、碱对活性炭进行调变处理，通过 XRF、BET、Boehm 滴定、GC-MS 等对处理前后活性炭的物理结构、表面基团、无机氧化物种类和数量，以及反应后活性炭的物理结构和表面残留有机物的表征分析，研究了活性炭催化TeCA脱HCl反应性能与其表面物化性质的对应关系。结果表明：酸、碱等处理对活性炭物理结构和表面基团影响较小，但显著改变了无机氧化物种类和数量；反应后活性炭比表面积下降明显，表面残留有五氯丁二烯；活性炭中铝、铁氧化物与五氯丁二烯含量、孔道堵塞程度和失活速率呈密切对应关系。铝、铁与HCl生成的AlCl3和FeCl3 Lewis酸中心是促进TCE聚合进而导致孔道堵塞而失活的主要原因。
활성탄표면물화성질시탄기최화제최화TeCA탈HCl합성TCE반응성능적중요영향인소。채용산、감대활성탄진행조변처리，통과 XRF、BET、Boehm 적정、GC-MS 등대처리전후활성탄적물리결구、표면기단、무궤양화물충류화수량，이급반응후활성탄적물리결구화표면잔류유궤물적표정분석，연구료활성탄최화TeCA탈HCl반응성능여기표면물화성질적대응관계。결과표명：산、감등처리대활성탄물리결구화표면기단영향교소，단현저개변료무궤양화물충류화수량；반응후활성탄비표면적하강명현，표면잔류유오록정이희；활성탄중려、철양화물여오록정이희함량、공도도새정도화실활속솔정밀절대응관계。려、철여HCl생성적AlCl3화FeCl3 Lewis산중심시촉진TCE취합진이도치공도도새이실활적주요원인。
The physical and chemical properties of the activated carbon have an important influence on the performance of carbon based catalysts for the dehydrochlorination reaction of tetrachloroethane(TeCA) to trichloroethylene (TCE). Activated carbons were pretreated by the use of acid or alkali solution. The surface oxygen-containing groups, physical structure, and the types and content of inorganic oxides of untreated and pretreated activated carbons were characterized by XRF, BET and Boehm titration. The physical structure and high boiling organic residues of the used activated carbon samples were obtained with the help of BET and GC-MS. The performances of different treated activated carbon samples for the reaction of TeCA to TCE were investigated. Furthermore, deactivation mechanism was discussed by the association of these physical and chemical properties and the stability of the activated carbon samples. The results showed that the treatments brought major change to the type and content of inorganic oxides rather than oxygen-containing groups and physical structure. The specific surface area and pore volume of the used carbon samples decreased with the generated 1,1,2,4,4-pentachlorobuta-1,3-diene. The main factor on the stability of activated carbon samples was not the surface oxygenic groups, but the Al and Fe. Water and Lewis acid like AlCl3 and FeCl3 were generated <br> from the reaction of Al (Fe) oxides and by-product HCl. Under the effect of the Lewis acid,tetrachloroethane or trichloroethylene accelerates the formation of carbocation intermediate. Then, carbocation was polymerized with trichloroethene and undergone dehydrochlorination to give 1,1,2,4,4-pentachlorobuta-1,3-diene (1,1,2,3,4-pentachlorobuta-1,3-diene), even other polymerizations with longer molecular chains. These polymers were accumulated in the hole of activated carbon, leading to the decrease of the specific surface area and then the deactivation of the catalyst.