Pd-K/MgAlO催化剂上的NOx存储、脱附和还原过程

张业新, 王晓, 王力, 王仲鹏, 李倩, 张昭良. Pd-K/MgAlO催化剂上的NOx存储、脱附和还原过程[J]. 环境化学, 2013, 32(7): 1300-1307. doi: 10.7524/j.issn.0254-6108.2013.07.025
引用本文: 张业新, 王晓, 王力, 王仲鹏, 李倩, 张昭良. Pd-K/MgAlO催化剂上的NOx存储、脱附和还原过程[J]. 环境化学, 2013, 32(7): 1300-1307. doi: 10.7524/j.issn.0254-6108.2013.07.025
ZHANG Yexin, WANG Xiao, WANG Li, WANG Zhongpeng, LI Qian, ZHANG Zhaoliang. NOx storage, desorption and reduction over Pd-K/MgAlO catalyst[J]. Environmental Chemistry, 2013, 32(7): 1300-1307. doi: 10.7524/j.issn.0254-6108.2013.07.025
Citation: ZHANG Yexin, WANG Xiao, WANG Li, WANG Zhongpeng, LI Qian, ZHANG Zhaoliang. NOx storage, desorption and reduction over Pd-K/MgAlO catalyst[J]. Environmental Chemistry, 2013, 32(7): 1300-1307. doi: 10.7524/j.issn.0254-6108.2013.07.025

Pd-K/MgAlO催化剂上的NOx存储、脱附和还原过程

  • 基金项目:

    国家高技术研究发展计划(863)(2008AA06Z320)

    国家自然科学基金(21077043,21277060)

    山东省博士基金(BS2011HZ002)资助.

NOx storage, desorption and reduction over Pd-K/MgAlO catalyst

  • Fund Project:
  • 摘要: 利用程序升温脱附(TPD)、程序升温表面反应(TPSR)和原位红外光谱(in situ IR)等技术研究了Pd-K/MgAlO催化剂上的NOx存储、脱附和还原过程.结果表明,NOx在Pd-K/MgAlO上主要以硝酸根和亚硝酸根的形式存储.在Pd的催化作用下,部分亚硝酸根被氧化为强酸性的硝酸根,变得更容易存储.由NOx-TPD计算得到Pd-K/MgAlO的NOx存储容量高达890.4 μmol·g-1.此外,在NOx脱附及H2还原的实验中均发现了Pd催化的亚硝酸盐歧化分解反应,该反应通过亚硝酸盐溢流至Pd位实现.亚硝酸盐的溢流产生了两个作用:促进NOx低温脱附及促进H2对存储NOx的还原.此发现为NOx存储物种的溢流机理提供了一个有力的证据.
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  • 收稿日期:  2012-12-01
张业新, 王晓, 王力, 王仲鹏, 李倩, 张昭良. Pd-K/MgAlO催化剂上的NOx存储、脱附和还原过程[J]. 环境化学, 2013, 32(7): 1300-1307. doi: 10.7524/j.issn.0254-6108.2013.07.025
引用本文: 张业新, 王晓, 王力, 王仲鹏, 李倩, 张昭良. Pd-K/MgAlO催化剂上的NOx存储、脱附和还原过程[J]. 环境化学, 2013, 32(7): 1300-1307. doi: 10.7524/j.issn.0254-6108.2013.07.025
ZHANG Yexin, WANG Xiao, WANG Li, WANG Zhongpeng, LI Qian, ZHANG Zhaoliang. NOx storage, desorption and reduction over Pd-K/MgAlO catalyst[J]. Environmental Chemistry, 2013, 32(7): 1300-1307. doi: 10.7524/j.issn.0254-6108.2013.07.025
Citation: ZHANG Yexin, WANG Xiao, WANG Li, WANG Zhongpeng, LI Qian, ZHANG Zhaoliang. NOx storage, desorption and reduction over Pd-K/MgAlO catalyst[J]. Environmental Chemistry, 2013, 32(7): 1300-1307. doi: 10.7524/j.issn.0254-6108.2013.07.025

Pd-K/MgAlO催化剂上的NOx存储、脱附和还原过程

  • 1.  济南大学化学化工学院, 济南, 250022;
  • 2.  中国科学院宁波材料技术与工程研究所, 宁波, 315201
基金项目:

国家高技术研究发展计划(863)(2008AA06Z320)

国家自然科学基金(21077043,21277060)

山东省博士基金(BS2011HZ002)资助.

摘要: 利用程序升温脱附(TPD)、程序升温表面反应(TPSR)和原位红外光谱(in situ IR)等技术研究了Pd-K/MgAlO催化剂上的NOx存储、脱附和还原过程.结果表明,NOx在Pd-K/MgAlO上主要以硝酸根和亚硝酸根的形式存储.在Pd的催化作用下,部分亚硝酸根被氧化为强酸性的硝酸根,变得更容易存储.由NOx-TPD计算得到Pd-K/MgAlO的NOx存储容量高达890.4 μmol·g-1.此外,在NOx脱附及H2还原的实验中均发现了Pd催化的亚硝酸盐歧化分解反应,该反应通过亚硝酸盐溢流至Pd位实现.亚硝酸盐的溢流产生了两个作用:促进NOx低温脱附及促进H2对存储NOx的还原.此发现为NOx存储物种的溢流机理提供了一个有力的证据.

English Abstract

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