中性条件Fe/Cu-MCM-41光催化活化H_(2)O_(2)/PDS的构-效关系  

The structure-activity relationship of Fe/Cu-MCM-41 on photocatalytic activation of H_(2)O_(2)/PDS under neutral condition

作　　者：张传波 熊志超 邓佩 刘力章 冯斐[1,2] 邵莉[1,2] 陈建新[1,2] ZHANG Chuanbo;XIONG Zhichao;DENG Pei;LIU Lizhang;FENG Fei;SHAO Li;CHEN Jianxin(School of Resources&Environment,Nanchang University,Nanchang,330031,China;The Key Laboratory of Poyang Lake Environment and Resource Utilization,Ministry of Education,Nanchang University,Nanchang,330031,China;Jiangxi Academy of Eco-Environmental Sciences and Planning,Nanchang,330077,China)

机构地区：[1]南昌大学资源与环境学院,南昌330031 [2]南昌大学鄱阳湖环境与资源利用教育部重点实验室,南昌330031 [3]江西省生态环境科学研究与规划院,南昌330077

出　　处：《环境化学》2024年第6期2036-2046,共11页Environmental Chemistry

基　　金：国家自然科学基金(21966021,21367021);广东省科技计划(2020B1212060055)资助.

摘　　要：本文在室温下制备了Fe-MCM-41和Cu-MCM-41,利用XRD、BET、SEM和TEM等手段对催化剂进行了表征.选取金橙Ⅱ为探针分子、H_(2)O_(2)和PDS作为氧化剂,构建了多相光催化氧化体系,研究中性条件下Fe-MCM-41和Cu-MCM-41光催化活化H_(2)O_(2)和PDS的构-效关系.结果表明,Fe-MCM-41为同晶替换型催化剂,Cu-MCM-41为同晶替换和CuO孤岛共存型催化剂.中性条件下,H_(2)O_(2)受空间位阻和电性排斥影响小,能被Fe-MCM-41孔道内外铁离子高效光催化产生·OH,但难以被Cu-MCM-41中同晶替换和孤岛的铜离子高效光催化;PDS由于受到空间位阻和电性排斥的影响,难以进入Fe-MCM-41和Cu-MCM-41孔道之中,但Cu-MCM-41表面和孤岛上的铜离子能高效光催化PDS产生^(1)O_(2)和SO_(4)^(−·)·UV+H_(2)O_(2)体系中加入Fe-MCM-41,金橙Ⅱ的脱色速率提升了52.9%,反应180 min时体系矿化率从43%提高到了57%;UV+PDS体系中加入Cu-MCM-41,金橙Ⅱ的脱色速率提升了38.7%,反应180 min时体系矿化率从48%提高到了76%.本研究为介孔分子筛光催化剂的开发利用提供理论依据.In this study,Fe-MCM-41 and Cu-MCM-41 were synthesized at room temperature and were characterized by XRD,BET,SEM and TEM techniques.In the heterogeneous photocatalytic oxidation system,Fe-MCM-41 and Cu-MCM-41,OrangeⅡ,H_(2)O_(2) and PDS were selected as catalysts,modal pollutant and oxidants,respectively.The structure-activity relationship of Fe-MCM-41 and Cu-MCM-41 on photocatalytic activation of H_(2)O_(2) and PDS under neutral condition was discussed.The results showed that the configuration of Fe-MCM-41 was isomorphous substitution,and the configuration of Cu-MCM-41 was isomorphous substitution coexisting with CuO island.Under neutral condition,it was easy for H_(2)O_(2) to enter the pore of Fe-MCM-41 or Cu-MCM-41 since H_(2)O_(2) was less influenced by steric hindrance and electrical repulsion.·OH could be efficiently generated through H_(2)O_(2) photo-activation by iron ions inside and outside the pore of Fe-MCM-41,but it was difficult for H_(2)O_(2) to be efficiently catalyzed by copper ions in Cu-MCM-41.It was hard for PDS to enter the pore of Fe-MCM-41 or Cu-MCM-41 due to the higher steric hindrance and electrical repulsion under neutral condition,but the copper ions on the surface of Cu-MCM-41 and CuO island could efficiently photo-activate PDS to produce ^(1)O_(2) and SO_(4)^(−·)·When Fe-MCM-41 was added into UV+H_(2)O_(2) system,the enhanced efficiency of OrangeⅡdecolorization rate could reach 52.9%,and its mineralization increased from 43%to 57%at 180 min.When Cu-MCM-41 was added into UV+PDS system,the enhanced efficiency of OrangeⅡdecolorization rate could reach 38.7%,and its mineralization increased from 48%to 76%at 180 min.This study provided a theoretical basis for the development and utilization of mesoporous molecular sieve photocatalysts.

关 键 词：MCM-41 过氧化氢 过二硫酸盐 光催化活化 构-效关系 

分 类 号：X-1[环境科学与工程] O6[理学—化学]