La2O3掺入对提升CuMnOx/堇青石催化氧化氯苯性能的研究OA
The enhancement of CuMnOx/Cordierite catalytic oxidation of chlorobenzene by La2O3 doping
含氯挥发性有机物(Cl-VOCs)由于来源广泛、毒性强、不易降解、易产生多氯副产物等特点,环境危害大,备受人们高度关注.催化氧化技术因其起燃温度低、能耗小、效率高、无二次污染等优点,已成为当前Cl-VOCs处理主流技术和发展方向.本研究通过柠檬酸络合法制备了一系列氧化镧(La2O3)掺入的CuMnOx/堇青石催化剂催化氧化氯苯,考察了Cu/Mn摩尔比、La2O3 掺入量、CuMnOx负载量以及煅烧温度对催化剂氧化性能影响,并采用X射线衍射(XRD)、布鲁诺-埃梅特-泰勒法(BET)、氢气程序升温还原(H2-TPR)、氧气程序升温脱附(O2-TPD)、X射线光电子能谱(XPS)、原位漫反射傅里叶变换红外光谱(in-situ DRIFTs)等分析手段对催化剂理化性质进行分析.结果发现,La2O3 的掺入显著提升催化剂氧化活性,且随着掺入量的增加,H2 还原峰温度逐渐降低,也有利于的O−脱附,更高效地提供活性氧,经 500℃煅烧所制CuMn3LaOx/堇青石最佳,T99=300℃,CuMn2O4、MnO2 和La2O3 间的协同作用,即Cu2+/Cu、Mn4+/Mn3+和La3+/La间的氧迁移是该催化剂具有良好性能的重要原因,且催化剂高比表面积和孔体积进一步提升了其氧化活性.同时,研究考察了催化剂重复性、稳定性以及可能的氧化机理,催化剂展示出良好的催化剂稳定性,未发现催化中毒失活现象的发生.
Chlorine-containing volatile organic compounds(Cl-VOCs)pose significant environmental risks and have received considerable attention due to their widespread sources,strong toxicity,difficulty in degradation,and the tendency to produce polychlorinated by-products.Among current treatment methods,catalytic oxidation technology has emerged as the dominant approach for Cl-VOC removal,owing to its advantages such as low ignition temperature,low energy consumption,high efficiency and absence of secondary pollution.In this study,a series of CuMnOx/cordierite catalysts doped with La2O3 were prepared using the citric acid complexation method for the catalytic oxidation of chlorobenzene.The effects of the molar ratio of Cu/Mn,the incorporation amount of La2O3,the loading of CuMnOx and the calcination temperature on the oxidation performance of the catalysts were investigated.The physicochemical properties of the catalyst were characterized by XRD,BET,H2-TPR,O2-TPD,XPS,and in-situ DRIFTs techniques.The results revealed that the addition of La2O3 significantly enhanced the oxidation activity of the catalyst,with performance improving as the doping concentration increased.The temperature of the H2 reduction peak gradually decreased,facilitating O-desorption and promoting the generation of active oxygen.The CuMn3LaOx/cordierite prepared by calcination at 500℃exhibited the highest performance,with T99=300℃.The synergistic effect among CuMn2O4,MnO2 and La2O3,namely the oxygen migration among Cu2+/Cu,Mn4+/Mn3+and La3+/La,was an important reason for the good performance of this catalyst,and the high specific surface area and pore volume of the catalyst further enhancd its oxidation activity.Meanwhile,the repeatability,stability and possible oxidation mechanism of the catalyst were investigated.The catalyst demonstrated good stability throughout testing,with no evidence of catalytic deactivation or poisoning.
单佳鑫;黄琼;杨孜素;童熙;毛君杰;魏琛;杨波;李大伟;陶涛
江苏省大气环境与装备技术协同创新中心,江苏省大气环境监测与污染控制高技术研究实验室,南京信息工程大学环境科学与工程学院,南京 210044江苏省大气环境与装备技术协同创新中心,江苏省大气环境监测与污染控制高技术研究实验室,南京信息工程大学环境科学与工程学院,南京 210044江苏省大气环境与装备技术协同创新中心,江苏省大气环境监测与污染控制高技术研究实验室,南京信息工程大学环境科学与工程学院,南京 210044江苏省大气环境与装备技术协同创新中心,江苏省大气环境监测与污染控制高技术研究实验室,南京信息工程大学环境科学与工程学院,南京 210044江苏省大气环境与装备技术协同创新中心,江苏省大气环境监测与污染控制高技术研究实验室,南京信息工程大学环境科学与工程学院,南京 210044江苏省大气环境与装备技术协同创新中心,江苏省大气环境监测与污染控制高技术研究实验室,南京信息工程大学环境科学与工程学院,南京 210044江苏省大气环境与装备技术协同创新中心,江苏省大气环境监测与污染控制高技术研究实验室,南京信息工程大学环境科学与工程学院,南京 210044江苏省大气环境与装备技术协同创新中心,江苏省大气环境监测与污染控制高技术研究实验室,南京信息工程大学环境科学与工程学院,南京 210044南京信息工程大学化学与材料学院,南京 210044
资源环境
催化氧化含氯挥发性有机物氧化镧柠檬酸络合法堇青石
catalytic oxidationchlorinated volatile organic compoundslanthanum oxidecitric acid complex methodcordierite
《环境工程学报》 2026 (1)
157-166,10
国家自然科学基金资助项目(21501097、51902166、52000101)江苏省自然科学基金资助项目(BK20170954、BK20150890、BK20190786)江苏省高等学校"青蓝工程"和江苏省高等学校重点学科建设项目资助项目(PAPD)
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