臭氧协同Fe/SSZ-13分子筛催化氧化低浓度甲烷的性能研究

桂煜,周光照,李佩青,陈婷,李珂,林赫

车用发动机 ›› 2023, Vol. 0 ›› Issue (2) : 1-10.

车用发动机 ›› 2023, Vol. 0 ›› Issue (2) : 1-10.
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臭氧协同Fe/SSZ-13分子筛催化氧化低浓度甲烷的性能研究

  • 桂煜1,周光照1,李佩青2,陈婷1,李珂2,林赫1
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Catalytic Oxidation of Low-Concentration Methane by Ozone-Assisted Fe/SSZ-13 Zeolite

  • GUI Yu1,ZHOU Guangzhao1,LI Peiqing2,CHEN Ting1,LI Ke2,LIN He1
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摘要

当前低浓度甲烷催化氧化存在起燃温度高、贵金属用量大等问题,为探索低成本、清洁高效的甲烷去除技术,基于臭氧的强氧化性和Fe/SSZ-13分子筛优异的吸附性,探究了在臭氧(O3)气氛下Fe负载量、n(CH4)∶n(O3)以及空速对甲烷催化氧化性能的影响。研究结果表明,在Fe负载量为1%,n(CH4)∶n(O3)为1∶6,温度为200 ℃的条件下,甲烷的转化率可达80.8%。通过BET,XRD,NH3-TPD,H2-TPR,UV-Vis以及XPS表征手段,证明了适量的Fe负载可以提高催化剂比表面积,促进更多酸性位点的形成,调节催化剂表面铁元素的价态分布和种类,从而促进甲烷催化臭氧化反应。基于原位红外试验发现O3可以活化活性位点,进而促进甲烷吸附和催化氧化反应。

Abstract

At present, for the catalytic oxidation of lowconcentration methane, there exist the problems such as high ignition temperature and large consumption of precious metals. In order to explore a lowcost, clean and efficient methane removal technology, the effects of Fe loading, O3/CH4 and space velocity on catalytic oxidation of methane were investigated based on the strong oxidation of ozone and the excellent adsorption of Fe/SSZ-13 zeolite. The research results show that the methane conversion rate can reach 80.8% under the conditions of 1% Fe loading, CH4/O3=16 and 200 reaction temperature. By means of BET, XRD, NH3-TPD, H2-TPR, UV-Vis and XPS, Fe loading is proved to be able to increase the specific surface area of catalyst, promote the formation of more acidic sites and regulate the valence distribution and species of iron on the catalyst surface, which promotes catalytic ozonation of methane. According to insitu infrared test, O3 can activate active sites and hence promote methane adsorption and catalytic oxidation.

关键词

甲烷 / 催化氧化 / 臭氧 / 分子筛

Key words

methane / catalytic oxidation / ozonation / molecular sieve

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桂煜,周光照,李佩青,陈婷,李珂,林赫. 臭氧协同Fe/SSZ-13分子筛催化氧化低浓度甲烷的性能研究[J]. 车用发动机. 2023, 0(2): 1-10
GUI Yu,ZHOU Guangzhao,LI Peiqing,CHEN Ting,LI Ke,LIN He. Catalytic Oxidation of Low-Concentration Methane by Ozone-Assisted Fe/SSZ-13 Zeolite[J]. Vehicle Engine. 2023, 0(2): 1-10

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