低温等离子体耦合Co-Mn双金属催化剂降解三氯乙烯  

Removal of trichloroethylene by non-thermal plasma combined with Co-Mn bimetallic catalyst

作　　者：侯浩 党小庆[1,2] 李世杰 于欣 王鹏勇 孟祥康 HOU Hao;DANG Xiaoqing;LI Shijie;YU Xin;WANG Pengyong;MENG Xiangkang(School of Environment&Municipal Engineering,Xi'an University of Architecture&Technology,Xi'an,710055,China;Key Laboratory of Environmental Engineering of Shaanxi Province,Xi'an,710055,China)

机构地区：[1]西安建筑科技大学环境与市政工程学院,西安710055 [2]陕西省环境工程重点实验室,西安710055

出　　处：《环境化学》2023年第4期1185-1195,共11页Environmental Chemistry

基　　金：国家重点研发计划课题(2017YFC0212204);陕西省重点研发计划(2018ZDCXL-SF-02-04)资助.

摘　　要：以γ-Al_(2)O_(3)为载体,采用等体积浸渍法制备钴锰催化剂(Co/γ-Al_(2)O_(3)、Mn/γ-Al_(2)O_(3)、Co_(3)Mn_(1)/γ-Al_(2)O_(3)、Co_(1)Mn_(1)/γ-Al_(2)O_(3)、Co_(1)Mn_(3)/γ-Al_(2)O_(3)),研究不同催化剂耦合低温等离子体(NTP)对三氯乙烯的降解性能.与单一NTP相比,NTP耦合催化剂可显著提高三氯乙烯的去除率、COx产率、碳平衡、HCl和Cl2产率,减少副产物的产生.Co-Mn双金属催化剂催化性能高于单一Co和Mn负载的催化剂,其中Co_(3)Mn_(1)/γ-Al_(2)O_(3)具有最高的催化活性,电压为6—10 kV,Co_(3)Mn_(1)/γ-Al_(2)O_(3)耦合NTP对三氯乙烯去除率(39.7%—96.94%)与COx(33.04%—87.36%)产率最高.通过BET、XRD、H2-TPR、XPS表征催化剂的物化性质,以阐明不同催化剂耦合NTP降解三氯乙烯效果存在差异的原因.结果显示,Co_(3)Mn_(1)/γ-Al_(2)O_(3)催化剂具有较高的比表面积,较小的Co_(3)O_(4)晶粒尺寸,较低的还原温度,且催化剂表面上的Mn^(4+)、Co_(3+)和Oads含量更高,有利于三氯乙烯的降解.最后通过GC-MS分析三氯乙烯降解过程中产生的有机中间体,推测了低温等离子体降解三氯乙烯的反应路径.The cobalt-manganese catalysts(Co/γ-Al_(2)O_(3)、Mn/γ-Al_(2)O_(3)、Co_(3)Mn_(1)/γ-Al_(2)O_(3)、Co_(1)Mn_(1)/γ-Al_(2)O_(3)、Co_(1)Mn_(3)/γ-Al_(2)O_(3))were prepared by equal volume impregnation method usingγ-Al_(2)O_(3) as the carrier to study the degradation performance of trichloroethylene by different catalysts coupled with non-thermal plasma(NTP).Compared with single NTP,the NTP-coupled catalyst significantly improved the removal of trichloroethylene、COx yield、Carbon balance、HCl and Cl2 yield、and reduced by-product generation.The catalytic performance of Co-Mn bimetallic catalysts is higher than that of single Co and Mn loaded catalysts,and Co_(3)Mn_(1)/γ-Al_(2)O_(3) has the highest catalytic activity.At the voltage of 6—10 kV,Co_(3)Mn_(1)/γ-Al_(2)O_(3) coupled with NTP has the highest removal rate of trichloroethylene(39.7%—96.94%)and the highest COx yield(33.04%—87.36%).BET、XRD、H2-TPR、XPS were used to characterize the physical and chemical properties of the catalysts to clarify the reasons for the differences in the performance of different catalysts coupled with NTP in the degradation of trichloroethylene.The results showed that the Co_(3)Mn_(1)/γ-Al_(2)O_(3) catalyst had higher specific surface area,smaller Co_(3)O_(4) grain size,lower reduction temperature,and higher content of Mn^(4+)、Co_(3+)and Oads on the catalyst surface,which were beneficial to the degradation of trichloroethylene.Finally,the organic intermediates produced during the degradation of trichloroethylene were analyzed by GC-MS to speculate the reaction path of trichloroethylene degradation by non-thermal plasma.

关 键 词：低温等离子体 钴锰双金属催化剂 三氯乙烯 去除率 副产物 

分 类 号：X701[环境科学与工程—环境工程] TQ426[化学工程]