摘要
以前驱体浸渍法制备铜基碳材料(Cu/AC)为催化剂,考察固定床反应器中不同操作条件对催化湿式氧化(CWAO)降解苯酚性能的影响。利用N_(2)-吸附脱附、XRD、XPS、热重技术,对反应前后Cu/AC结构进行表征,探究Cu/AC失活原因。结果表明,Cu/AC催化CWAO反应的最优操作条件为反应温度180℃,反应压力3.0 MPa,液时空速15 mL(g·h),气时空速4.5 L/(g·h),在反应5 h时苯酚、化学需氧量(COD)转化率分别达到97.0%、89.4%。Cu/AC催化剂失活的原因主要为Cu组分流失和表面沉积物的生成。反应过程中,Cu^(+)和Cu^(0)被氧化为更易流失的Cu^(2+),导致Cu组分流失,降低催化活性;此外,部分中间产物沉积在Cu/AC表面,造成催化剂孔道堵塞,暴露的活性位点减少,使得催化活性进一步降低。
Utilizing Cu-based carbon materials(Cu/AC)prepared by precursor impregnation method as catalysts,the effects of different operating conditions on the performance of catalytic wet oxidation(CWAO)degradation of phenol were investigated in a fixedbed reactor.The structures of fresh and used Cu/AC were characterized by N_(2)-adsorption desorption,XRD,XPS,and TG to study the main reasons for the deactivation of Cu/AC catalysts.The results showed that the optimum operating conditions of Cu/AC were reaction temperature of 180℃,reaction pressure of 3.0 MPa,liquid hourly space velocity of 15 mL/(g·h),and gas hourly space velocity of 4.5 L/(g·h).Under the optimum conditions,Cu/AC catalyst achieved 97.0%of phenol conversion and 89.4%of chemical oxygen demand(COD)conversion after a reaction time of 5 h.The deactivation of Cu/AC could be attributed to the loss of Cu species and surface deposition.During reaction process,Cu^(+)and Cu^(0)were trended to be oxidized to Cu^(2+),which was more easily leached into the solution.Consequently,the gradual loss of Cu species resulted in a decrease in the catalytic activity of Cu/AC.Additionally,the surface of Cu/AC was covered by partial intermediate products to block the micropores,further reducing the number of exposed active sites and catalytic activity.
作者
王宏宇
裴永丽
张莹
喻泽华
栗俊田
WANG Hong-yu;PEI Yong-li;ZHANG Ying;YU Ze-hua;LI Jun-tian(Department of Energy Chemistry and Materials Engineering,Shanxi Institute of Energy,Jinzhong 030600,China)
出处
《化学研究与应用》
CAS
北大核心
2024年第8期1810-1818,共9页
Chemical Research and Application
基金
山西省基础研究计划项目(202303021222296)资助
山西省高等学校科技创新项目(2022L605)资助。
关键词
苯酚废水
催化湿式氧化
Cu/AC
操作条件
失活
phenol wastewater
catalytic wet oxidation
Cu-based carbon catalyst
operating condition
deactivation
作者简介
通讯联系人:王宏宇(1992-),男,讲师,主要从事污染物控制化学研究。E-mail:wanghy@sxie.edu.cn。
