研究报告
蒋和雁,吴豪,胡志德,边凤霞.温和条件下磁性Pd-MgFe2O4/MgAl(O)催化4-氯苯酚高效加氢脱氯[J].环境科学学报,2021,41(3):969-979
温和条件下磁性Pd-MgFe2O4/MgAl(O)催化4-氯苯酚高效加氢脱氯
- Magnetic Pd-MgFe2O4/MgAl(O) catalyzed highly efficient hydrodechlorination of 4-chlorophenol under mild conditions
- 基金项目:重庆市自然科学基金(No.cstc2018jcyjAX0735,cstc2019jcyj-msxmX0641);国家自然科学基金(No.21201184);重庆市教委自然科学基金(No.KJQN201900811);重庆工商大学自然科学基金(No.950119090);催化与环境新材料重庆市重点实验室项目(No.KFJJ2019082);重庆市高等学校“十三五”市级化学工程与技术重点学科资助项目
- 蒋和雁
- 重庆工商大学环境与资源学院, 重庆高校催化理论与应用技术市级重点实验室, 催化与环境新材料重庆市重点实验室, 重庆 400067
- 吴豪
- 重庆工商大学环境与资源学院, 重庆高校催化理论与应用技术市级重点实验室, 催化与环境新材料重庆市重点实验室, 重庆 400067
- 胡志德
- 陆军勤务学院军事设施系, 重庆 401331
- 边凤霞
- 重庆工商大学环境与资源学院, 重庆高校催化理论与应用技术市级重点实验室, 催化与环境新材料重庆市重点实验室, 重庆 400067
- 摘要:以镁铁尖晶石MgFe2O4为磁核,在磁核表层包覆MgAl水滑石后经高温焙烧形成MgAl (O)复合氧化物包覆的磁性载体MgFe2O4/MgAl (O),进而负载纳米金属Pd制成磁性催化剂Pd-MgFe2O4/MgAl (O).通过X射线衍射(XRD)、X射线光电子能谱分析(XPS)、傅里叶红外光谱(FT-IR)、透射电镜(TEM)、扫描电子显微镜(SEM)、选区电子衍射(SAED)、比表面积(SBET)和振动样品磁强计(VSM)等手段对催化材料进行表征.结果表明,MgFe2O4-LDH转化为磁性MgFe2O4/MgAl (O)载体有利于催化材料比表面积的增加、结构稳定性的提升及相应催化活性位点的增加,进而有利于提升4-氯苯酚高效加氢脱氯效率.研究进一步考察了催化剂负载量、催化剂用量、底物浓度、反应温度、反应溶剂等条件对4-氯苯酚降解效率的影响.结果发现,在优化反应条件下催化反应的转换频率TOF (0.04 s-1)可媲美常温、常压、无碱性添加剂等温和条件下4-氯苯酚高效加氢脱氯反应的最佳文献报道水平.磁性催化剂Pd-MgFe2O4/MgAl (O)循环使用4次后仍保持很好的催化活性.
- Abstract:The MgFe2O4 was used as the magnetic core,which was coated with MgAl hydrotalcite.After high-temperature calcination, MgAl(O) compound oxide based magnetic carrier MgFe2O4/MgAl(O) was formed.Magnetic catalyst Pd-MgFe2O4/MgAl(O) was prepared by nano-metal Pd loading.The material were characterized by X-ray diffraction(XRD),X-ray photoelectron spectroscopy (XPS),fourier infrared spectroscopy(FT-IR),transmission electron microscopy(TEM),scanning electron microscopy(SEM),selected area electron diffraction(SAED),brunauer emmett teller method(SBET) and vibrating sample magnetometer(VSM) measurement.The study showed that the specific surface area,the structural stability and the corresponding catalytic active site of the catalytic material was enhanced by the transformation of MgFe2O4-LDH into the magnetic MgFe2O4/MgAl(O) carrier,which was beneficial to improve the efficiency of the hydrodechlorination of 4-chlorophenol.The removal efficiency of 4-chlorophenol was investigated under different conditions of catalyst loading,catalyst concentration,substrate concentration,reaction temperature as well as solvent.In comparison with literature,the TOF (0.04 s-1) of the catalytic 4-chlorophenol hydrodechlorination reaction under optimal reaction conditions approach one of the best efficiency under mild conditions such as room temperature,ambient pressure and no base additive.The catalytic efficiency of the magnetic catalyst Pd-MgFe2O4/MgAl(O) was well maintained after 4 recycle times.