研究报告

  • 肖远东,贾学辉,何丹,黄碧纯,杨颖欣,张勇,鲁美娟,涂翔,喻成龙.FeSAPO-34和CuFeSAPO-34分子筛的可控制备、表征及其低温NH3-SCR活性[J].环境科学学报,2022,42(6):357-368

  • FeSAPO-34和CuFeSAPO-34分子筛的可控制备、表征及其低温NH3-SCR活性
  • Controllable synthesis, characterization and low-temperature NH3-SCR activity of FeSAPO-34 and CuFeSAPO-34 molecular sieves
  • 基金项目:国家自然科学基金(No.51808269,52160009);江西省科技计划项目(No.20212BCJL23054,20192BAB203014,20201BBG71013); 国家重点研发计划(No.2019YFC1805804)
  • 作者
  • 单位
  • 肖远东
  • 江西农业大学国土资源与环境学院,南昌 330045
  • 贾学辉
  • 江西农业大学国土资源与环境学院,南昌 330045
  • 何丹
  • 江西农业大学国土资源与环境学院,南昌 330045
  • 黄碧纯
  • 华南理工大学环境与能源学院,广州 510006
  • 杨颖欣
  • 广东省环境科学研究院,广州 510045
  • 张勇
  • 江西农业大学国土资源与环境学院,南昌 330045
  • 鲁美娟
  • 江西农业大学国土资源与环境学院,南昌 330045
  • 涂翔
  • 江西省生态环境科学研究与规划院,南昌 330039
  • 喻成龙
  • 江西农业大学国土资源与环境学院,南昌 330045
  • 摘要:采用一锅水热法制备了一系列不同铁前驱体的FeSAPO-34分子筛催化剂和元素掺杂的分子筛催化剂,考察了铁源和元素掺杂对分子筛催化剂的可控合成和低温催化还原NOx性能的影响,并采用ICP、XRD、FESEM、BET、H2-TPR、XPS、NH3-TPD、EPR及UV-Vis DRS等表征技术进行分析.活性结果表明,不同铁前驱体对所制备的FeSAPO-34分子筛催化剂的可控合成产生较大影响且对应分子筛催化剂的NH3-SCR活性也存在较大差别.3种分子筛催化剂的低温活性顺序为:Fe0.1SAPO-34-C>Fe0.1SAPO-34-S>Fe0.1SAPO-34-N. Cu掺杂的Cu0.01Fe0.1SAPO-34催化剂在200 ℃时NOx转化率即可达82%,这反映出Cu掺杂能大大提高分子筛催化剂的低温选择性催化还原(SCR)活性.表征结果表明,不同铁源导致所制备催化剂的晶相结构、Fe物种类型及表面酸量等均存在较大差异.Cu0.01Fe0.1SAPO-34分子筛催化剂中孤立的铜离子物种为低温SCR反应提供了重要的活性中心.Cu掺杂的分子筛催化剂存在孤立的铜离子物种、具有丰富的表面酸性位及优异的氧化还原性能是其优异的低温NH3-SCR性能的重要原因.由此推测,Cu0.01Fe0.1SAPO-34催化剂在固定源低温烟气脱硝领域具有广阔应用前景.
  • Abstract:A series of FeSAPO-34 molecular sieve catalysts were prepared by a one-pot hydrothermal method employing different iron precursors and element doping. The effects of these parameters on the synthesis of the catalysts and their relative low temperature ammonia-selective catalytic reduction performance were investigated using ICP, XRD, FESEM, BET, H2-TPR, XPS, NH3-TPD, EPR, UV Vis DRS, and other methods. The results of the catalytic activity tests showed that choice of iron precursor had a significant influence on the synthesis of the FeSAPO-34 molecular sieve catalysts and on their relative activity for the NH3-SCR. The order of the activity of these catalysts at low temperatures was as follows: Fe0.1SAPO-34-C>Fe0.1SAPO-34-S>Fe0.1SAPO-34-N. The conversion of NOx by the Cu-doped Cu0.01Fe0.1SAPO-34 catalyst was 82% at 200 °C. This demonstrated that Cu doping greatly improved the low-temperature SCR activity of the Fe0.1SAPO-34 molecular sieve catalysts. The characterization results showed that different iron precursors led to great differences in the crystal structure, Fe species and surface acid content of the molecular sieve catalysts. The isolated Cu2+ species in Cu0.01Fe0.1SAPO-34 molecular sieve catalyst played an important role in NOx removal at low temperatures. The Cu doped molecular sieve catalysts had an isolated Cu2+ species, abundant surface acidic sites and excellent redox properties, which were important reasons for their excellent low temperature NH3-SCR activity. The Cu0.01Fe0.1SAPO-34 was shown to be a promising candidate as a SCR catalyst with great potential for low-temperature deNOx processes for stationary sources.

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