中性条件Fe/Cu-MCM-41光催化活化H2O2/PDS的构-效关系
The structure-activity relationship of Fe/Cu-MCM-41 on photocatalytic activation of H2O2/PDS under neutral condition
张传波 1熊志超 1邓佩 1刘力章 2冯斐 1邵莉 1陈建新1
作者信息
- 1. 南昌大学资源与环境学院,南昌,330031;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
- 2. 江西省生态环境科学研究与规划院,南昌,330077
- 折叠
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、H2O2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H2O2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,H2O2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1O2和SO4·.UV+H2O2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.
Abstract
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,Orange Ⅱ,H2O2 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 H2O2 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 H2O2 to enter the pore of Fe-MCM-41 or Cu-MCM-41 since H2O2 was less influenced by steric hindrance and electrical repulsion.OH could be efficiently generated through H2O2 photo-activation by iron ions inside and outside the pore of Fe-MCM-41,but it was difficult for H2O2 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 1O2 and SO4·.When Fe-MCM-41 was added into UV+H2O2 system,the enhanced efficiency of Orange Ⅱ decolorization 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 Orange Ⅱ decolorization 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Key words
MCM-41/H2O2/PDS/photocatalytic activation/structure-activity relationship引用本文复制引用
基金项目
国家自然科学基金(21966021)
国家自然科学基金(21367021)
广东省科技计划(2020B1212060055)
出版年
2024
NETL
NSTL
万方数据