四氯化碳与甲醇耦合原位加氢脱氯反应研究

项目名称： 四氯化碳与甲醇耦合原位加氢脱氯反应研究

项目编号： No.21307009

项目类型： 青年科学基金项目

立项/批准年度： 2014

项目学科： 环境科学、安全科学

项目作者： 鲁墨弘

作者单位： 常州大学

项目金额： 26万元

中文摘要： 四氯化碳对臭氧层有很强的破坏作用，通过催化加氢脱氯将CCl4转化为有用的产品是一种合理的处理方法。但加氢脱氯反应的强放热引起的活性组分烧结和生成的HCl对活性金属的毒化易使催化剂失活。本项目拟将强放热的CCl4加氢脱氯反应与吸热的甲醇水相重整反应耦合，降低反应热，避免催化剂局部温度过高而引起的烧结失活；同时，产生的HCl及时与甲醇在复合氧化物载体上反应，消除HCl对活性组分的毒化作用。采用既能活化CCl4，又能活化甲醇的Pd、Pt为活性组分，复合氧化物为载体，研究活性组分颗粒大小、负载量及表面氯覆盖度等对CCl4加氢脱氯与甲醇水相重整反应动态平衡的影响；研究载体酸碱性、表面覆盖度及载体改性等对HCl与甲醇反应性能的影响。阐明CCl4原位加氢脱氯反应和HCl与甲醇在载体上反应的机理，制备出高活性和稳定性的CCl4原位加氢脱氯催化剂，为含氯化合物加氢脱氯反应提供新的思路和理论依。

中文关键词： 四氯化碳；甲醇；耦合反应；原位；加氢脱氯

英文摘要： Carbon tetrachloride induces a very important environment problem by depleting the stratospheric ozone layer. An attractive way to eliminate CCl4 is to convert it into valuable intermediate products by catalytic hydrodechlorination. However, hydrodechlorination of CCl4 shows a rapid catalyst deactivation due to sintering caused by a high exothermicity of the reaction and poisoning by the produced HCl. The project studies the coupled reaction of hydrodechlorination of CCl4 and aqueous-phase reforming of methanol. Catalyst sintering can be avoided by the coupling of the high exothermic hydrodechlorination of CCl4 and endothermic aqueous-phase reforming of methanol for hydrogen generation. And the catalyst poisoning can be inhibited by the conversion of HCl to CH3Cl via the reaction with methanol on the catalyst support. Pd and Pt are employed as active metals supported on composite oxides due to their abilities to activate both CCl4 and methanol. The effect of particle size, loading of active metals and the Cl coverage on the catalyst surface on the coupled reaction is investigated. The influence of support properties on the reaction of HCl with methanol is also studied. The mechanism of the two reactions will be proposed and the catalysts with high activity and stability will be prepared.

英文关键词： CCl4；methanol；coupling reactions；in-situ；hydrodeclorination