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非晶态ZrO_2镶嵌的超细CeO_2催化HCl氧化
引用本文:徐希化,楼家伟,谢兴星,费兆阳,刘清,陈献,汤吉海,崔咪芬,乔旭.非晶态ZrO_2镶嵌的超细CeO_2催化HCl氧化[J].无机化学学报,2017,33(3):421-428.
作者姓名:徐希化  楼家伟  谢兴星  费兆阳  刘清  陈献  汤吉海  崔咪芬  乔旭
作者单位:南京工业大学材料化学工程国家重点实验室, 南京 210009;南京工业大学化工学院, 南京 210009,南京工业大学材料化学工程国家重点实验室, 南京 210009;南京工业大学化工学院, 南京 210009,南京工业大学材料化学工程国家重点实验室, 南京 210009;南京工业大学化工学院, 南京 210009,南京工业大学材料化学工程国家重点实验室, 南京 210009;南京工业大学化工学院, 南京 210009,南京工业大学材料化学工程国家重点实验室, 南京 210009;南京工业大学化工学院, 南京 210009,南京工业大学化工学院, 南京 210009,南京工业大学化工学院, 南京 210009,南京工业大学化工学院, 南京 210009,南京工业大学材料化学工程国家重点实验室, 南京 210009;南京工业大学化工学院, 南京 210009
基金项目:国家科技支撑计划(No.2011BAE18B01)、国家自然科学青年基金(No.21306089)和江苏省高校自然科学基金面上项目(No.13KJB530006)资助。
摘    要:采用不同方法制备了铈锆复合氧化物催化剂用于催化HCl氧化反应。自发沉积策略制备的CeO_2@ZrO_2催化剂中,超细CeO_2纳米粒子均匀的镶嵌于非晶态ZrO_2中。CeO_2粒子显著的"尺寸效应"使得该催化剂具有更高的Ce~(3+)和氧空位浓度,而较高的Ce~(3+)和氧空位浓度使得催化剂具有优异的低温氧化还原性能和储释氧能力。催化性能测试表明,CeO_2@ZrO_2催化剂展现出最好的催化活性(1.90 gCl2·gcat~(-1)·h~(-1)),同时CeO_2粒子周围非晶态的ZrO_2阻碍CeO_2的高温烧结,提高了该催化剂的稳定性。

关 键 词:催化氧化  氧化铈  氯循环  氧空位  尺寸效应
收稿时间:2016/8/29 0:00:00
修稿时间:2016/12/20 0:00:00

Superfine CeO2 Embedded in a Porous ZrO2 Matrix for Catalytic HCl Oxidation
XU Xi-Hu,LOU Jia-Wei,XIE Xing-Xing,FEI Zhao-Yang,LIU Qing,CHEN Xian,TANG Ji-Hai,CUI Mi-Fen and QIAO Xu.Superfine CeO2 Embedded in a Porous ZrO2 Matrix for Catalytic HCl Oxidation[J].Chinese Journal of Inorganic Chemistry,2017,33(3):421-428.
Authors:XU Xi-Hu  LOU Jia-Wei  XIE Xing-Xing  FEI Zhao-Yang  LIU Qing  CHEN Xian  TANG Ji-Hai  CUI Mi-Fen and QIAO Xu
Institution:State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 210009, China;College of Chemical Engineering, Nanjing Tech University, Nanjing 210009, China,State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 210009, China;College of Chemical Engineering, Nanjing Tech University, Nanjing 210009, China,State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 210009, China;College of Chemical Engineering, Nanjing Tech University, Nanjing 210009, China,State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 210009, China;College of Chemical Engineering, Nanjing Tech University, Nanjing 210009, China,State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 210009, China;College of Chemical Engineering, Nanjing Tech University, Nanjing 210009, China,College of Chemical Engineering, Nanjing Tech University, Nanjing 210009, China,College of Chemical Engineering, Nanjing Tech University, Nanjing 210009, China,College of Chemical Engineering, Nanjing Tech University, Nanjing 210009, China and State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 210009, China;College of Chemical Engineering, Nanjing Tech University, Nanjing 210009, China
Abstract:Ce-Zr composite oxide catalysts were prepared by different methods for catalytic HCl oxidation. The nano-sized CeO2 particles embedded in the amorphous ZrO2 matrix fabricated by spontaneous deposition strategy. A significant "size effect" of CeO2 nanoparticles leads to considerably high concentration of Ce3+ and oxygen vacancy sites, which makes the catalyst have excellent low-temperature oxidation reduction performance and oxygen storage capacity. Catalytic performance tests indicate that the CeO2@ZrO2 catalyst shows superior activity (1.90 gCL2·gcat-1·h-1) and good durability. The isolation of CeO2 nanoparticles by the amorphous ZrO2 is a key factor of durability of the catalyst.
Keywords:catalytic oxidation  CeO2  chlorine recycle  oxygen vacancy  size effect
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