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用浸渍法制备了一系列SiO_2负载的过渡金属催化剂M/SiO_2(M为第Ⅳ周期过渡金属),用于气相催化裂解1,1,2-三氯乙烷(TCE)脱HCl的反应。研究发现,在M/SiO_2催化剂中,Zn/SiO_2催化性能最好,TCE转化率能达到98%,顺-1,2-二氯乙烯(cis-DCE)的选择性为82%。随着Zn负载量的增加,Zn/SiO_2催化剂上TCE转化率逐渐增加,与催化剂上总酸量变化一致。将总酸量以Zn负载量归一化得到比酸量,则比酸量越大,Zn/SiO_2催化剂比活性越高,表明Zn/SiO_2催化剂表面酸性中心是TCE脱氯反应的活性中心。Zn/SiO_2催化剂在TCE脱HCl反应中存在一定的失活现象,归因于反应过程中催化剂表面积炭。低Zn负载量催化剂上会产生较多积炭,归因于其具有较多强酸性中心,表明催化剂表面强酸中心是导致催化剂积炭和失活的主要原因。
A series of SiO 2 supported transition metal catalysts, M / SiO 2 (M is transition metal Ⅳ), were prepared by impregnation method for the gas phase catalytic cracking of 1,1,2-trichloroethane (TCE). The results showed that the catalytic activity of Zn / SiO 2 was the best, the conversion of TCE reached 98% and the selectivity of cis-DCE was 82% in the M / SiO 2 catalyst. With the increase of Zn loading, the conversion of TCE on Zn / SiO 2 catalyst increased gradually, which was consistent with the change of total acid amount on the catalyst. The total acid amount was normalized by Zn loading to obtain the specific acid amount. The larger the specific acid amount, the higher the specific activity of the Zn / SiO 2 catalyst, indicating that the acidic center of the Zn / SiO 2 catalyst surface is the active center of the TCE dechlorination reaction. Zn / SiO 2 catalyst deactivation reaction in TCE there is a certain phenomenon, due to the catalyst surface during carbon deposition. The catalyst with low Zn loading will produce more coke, which is attributed to its more acidic sites, indicating that the strong acid sites on the catalyst surface are the main reasons for the catalyst coke and deactivation.