高分散性纳米级Fe0/BAC-cH2-t催化剂催化还原NO
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TQ426

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国家自然科学基金项目(面上项目,重点项目,重大项目)


Catalytic performance of highly dispersed nano-Fe0/BAC-cH2-t catalysts for catalytic reduction of NO by CO
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The National Natural Science Foundation of China (General Program, Key Program, Major Research Plan)

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    摘要:

    以椰壳活性炭为载体,采用氢气还原法制备出高分散性纳米级零价铁催化剂,采用固定床反应器研究了其对NO催化还原能力。采用XRD、TEM、SEM、XPS等分析手段对催化剂的微纳结构进行表征,考察了催化剂制备过程中H2浓度及煅烧还原温度对催化剂分散性、催化还原NO性能影响,催化剂的再生以及CO对催化剂还原NO的影响,并对CO还原NO反应机理进行推测。结果表明,催化剂活性随着H2浓度的增加逐渐增强,随着煅烧还原温度的升高先升高后降低。当H2浓度为100%时,在700℃煅烧温度下制备出的催化剂,Fe0粒径达到9 nm且均匀分散在椰壳活性炭中。Fe0/BAC-100H2-700催化剂在325℃时,NO转化率可以达到100%,表现出了良好的NO脱除效果。还原NO过程中,Fe0逐渐被氧化成Fe3O4导致催化剂最终失活,失活后的催化剂经再生处理后可恢复活性。NO还原反应过程中CO的加入可以还原Fe3O4再次生成Fe0,提供活性位点,有效的延长催化剂的寿命,减缓催化剂失活的速率。

    Abstract:

    Highly dispersed nano-zerovalent iron catalyst was prepared using hydrogen reduction method loaded on the activated carbon for NO reduction. The catalytic performance for catalytic reduction of NO was evaluated in a fixed-bed reactor. The catalysts were characterized by XRD, TEM, SEM, XPS and so on. The influence of H2 concentration and reduction temperature on the metal dispersion and NO removal performance of the catalyst were investigated, the regeneration of catalyst and the effect of CO on NO reduction were studied, and the CO-NO reaction mechanism was speculated. The results show that with the increase of H2 concentration, the activity of the catalyst was enhanced gradually. With the increase of preparation temperature, the activity of the catalyst was enhanced and then decreased. The particle size of Fe0/BAC-100H2-700 was 9 nm and Fe0 nanoparticles were evenly dispersed on the activated carbon. The NO removal performance of Fe0/BAC-100H2-700 catalyst could reach 100% at 325℃. In the process of NO removal, Fe0 was gradually oxidized to Fe3O4, leading to the deactivation of the catalyst. The deactivated catalyst can recover its activity after regeneration treatment. During the reaction, the addition of CO could reduce Fe3O4 to Fe0, increasing the life of catalyst and slow down the deactivation rate of catalyst effectively.

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王焕然,李先春,李丽,王思怡.高分散性纳米级Fe0/BAC-cH2-t催化剂催化还原NO[J].精细化工,2021,38(12):0

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  • 收稿日期:2021-06-18
  • 最后修改日期:2021-07-23
  • 录用日期:2021-07-26
  • 在线发布日期: 2021-10-08
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