CeO_(2)形貌对Ru/CeO_(2)液相催化还原N-二甲基亚硝胺的影响  

Effect of CeO_(2) morphology on Ru/CeO_(2) for liquid phase catalytic reduction of N-nitrosodimethylamine

作　　者：信晋凯 孙玉菡 余乐 郑寿荣[1] 许昭怡[1] XIN Jinkai;SUN Yuhan;YU Le;ZHENG Shourong;XU Zhaoyi(State Key Laboratory of Pollution Control and Resource Reuse Research,College of the Environment,Nanjing University,Nanjing,210023,China)

机构地区：[1]南京大学环境学院,污染控制与资源化研究国家重点实验室,南京210023

出　　处：《环境化学》2024年第11期3788-3797,共10页Environmental Chemistry

基　　金：国家自然科学基金(21976086)资助.

摘　　要：采用3种不同形貌的氧化铈(立方体c-CeO_(2)、棒状r-CeO_(2)与八面体o-CeO_(2))为载体,采用沉淀沉积法制备了Ru/CeO_(2)催化剂,并研究了水中N-二甲基亚硝胺(NDMA)的催化加氢还原反应.结果表明,3种催化剂的NDMA还原活性顺序为Ru/c-CeO_(2)>Ru/o-CeO_(2)>Ru/r-CeO_(2).XPS、拉曼等表征结果显示,Ru/c-CeO_(2)具有较高的Run+和适量的氧空位含量,其金属-载体相互作用最强,具有最高的还原活性.NDMA液相催化还原反应符合朗格缪尔-欣谢尔伍德模型,NDMA在催化表面的吸附是反应的控制步骤.催化剂对NDMA催化还原效率随着pH的升高呈倒火山型变化.催化剂经过5次循环利用后,仍有较好的催化活性.Ru/CeO_(2) catalysts were prepared by precipitation deposition method using three ceria oxides with different morphologies(cubic-CeO_(2),rod-CeO_(2) and octahedral-CeO_(2))as supports,and the catalytic hydrogenation reduction of N-dimethylnitrosamine(NDMA)was studied in water.The results show that the removal efficiency of NDMA on the three catalysts follows Ru/c-CeO_(2)>Ru/o-CeO_(2)>Ru/r-CeO_(2).The characterization results of XPS and Raman show that Ru/c-CeO_(2) has higher Run+and appropriate oxygen vacancy content,which has stronger metal support interaction and higher reduction activity than other catalysts.The NDMA liquid phase catalytic reduction reaction conforms to the Langmuir-Hinshelwood model,and the conversion of adsorbed NDMA on the catalytic surface is the rate-determining step.The liquid phase catalytic reduction of N-nitrosodimethylamine on Ru/CeO_(2) shows an inverted volcanic change with the increase of pH.The catalyst still has good catalytic activity after five cycles.

关 键 词：液相催化加氢 N-二甲基亚硝胺(NDMA) Ru/CeO_(2) 金属-载体相互作用 

分 类 号：X-1[环境科学与工程] O6[理学—化学]