Insight of platinum poisoning Cu/SAPO-34 during NH3-SCR and its promotion on catalysts regeneration after hydrothermal treatment

Insight of platinum poisoning Cu/SAPO-34 during NH3-SCR and its promotion on catalysts regeneration after hydrothermal treatment
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NH3-SCR过程中铂中毒Cu/SAPO-34的见解及其对水热处理后催化剂再生的促进作用

DOI:
10.1016/j.apcatb.2016.12.007
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发表时间:
2017-05
影响因子:
22.1
通讯作者:
Shen Meiqing
Shen Meiqing
中科院分区:
化学1区
文献类型:
--
作者:
Yu Tie;Xu Minhong;Huang Yu;Wang Jianqiang;Wang Jun;Lv Liangfang;Qi Gongshin;Li Wei;Shen Meiqing

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本文主要研究了氨选择性催化还原(NH3-SCR)脱除大气污染物NOx的反应,并采用一系列Pt浸渍Cu/SAPO-34(自制)样品,研究了其对脱NOx活性的负面影响以及水热处理对NH3-SCR活性复苏的促进作用。首先,通过XRD、NH_3-TPD和DRIFTs等方法研究了铂与沸石结构的相互作用以及对酸性的贡献。通过气体切换试验,分析了Pt对NH3-SCR活性的抑制作用,并总结了Pt对NH3-SCR反应网络(包括氨氧化、NO氧化和NO + NH3)的影响。H2-TPR和EPR进一步反映了Pt掺杂引起的各种Cu物种配位和氧化还原容量的变化。进一步的水热处理有利于Pt中毒的Cu/SAPO-34的再生,甚至在保持分子筛结构完整性的条件下,Pt的存在也有利于活性的提高。水热处理诱导铂烧结和STEM说明铂物种与铜氧化物结合并产生氧代络合物,削弱氨氧化。Pt的存在促进了水热处理过程中铜氧化物的进一步分散。最后总结了Cu/SAPO-34的铂中毒及水热处理后的再生情况,指出了其应用前景。
This study mainly focused on selective catalytic reduction of air pollutants NOxby ammonia (NH3-SCR), and a series of Pt impregnated Cu/SAPO-34 (homemade) samples were employed to elucidate its negative impact on DeNOxactivity and hydrothermal treatment’s acceleration on NH3-SCR activity resurgence. Firstly, XRD, NH3-TPD and DRIFTs were performed to examine platinum interaction with zeolites structure and contribution to acidity. Then, Pt inhibition on NH3-SCR activity was evaluated and its impact on reaction network, including ammonia oxidation, NO oxidation and NO + NH3, was concluded based on gas switching tests. H2-TPR and EPR further reflected various Cu species coordination and redox capacity variation caused by platinum doping. It was intriguing to find out that the further hydrothermal treatment benefited rejuvenation of Pt-poisoned Cu/SAPO-34 and even activity enhancement from Pt presence under the condition of zeolites structure integrity. Hydrothermal treatment induced platinum sintering and STEM illustrated platinum species combined with copper oxides and generated oxo-complexes, weakening ammonia oxidation. And Pt presence promoted copper oxides further dispersion during hydrothermal treatment. Finally, platinum poisoning on Cu/SAPO-34 and its regeneration after hydrothermal treatment were concluded to indicate their application potential.
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