等离子体制备稀土金属掺杂甲烷干气重整Ni/Mg/Al催化剂研究
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TQ426.6;TQ426.64;O643.32 2

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湖北省自然科学基金(批准号:2014CFB556)


Plasma Preparation of Rare-earthOxide Doped Ni/Mg/Al Catalyst for Dry Reforming of Methane
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    摘要:

    采用冷等离子体炬技术制备了以水滑石为前驱体的Ni/Mg/Al催化剂,考察了La和Ce助剂的添加对催化剂结构及其对CH4和CO2重整催化性能的影响。利用XRD、BET、XPS及TG对催化剂进行了表征和性能测试。结果表明:冷等离子体炬能快速分解Ni/Mg/Al水滑石前驱体,生成具有介孔特性的水镁石相Mg(Ni,Al)O固溶体,并生成Ni0晶粒。在温度700℃,空速30000mL/(h·gcat), V(CH4):V(CO2)=4:6的条件下,CH4和CO2的转化率分别为76%和61.8%。助剂Ce的添加增加了晶格氧,促进催化剂表面碳物种的消除,CH4和CO2的转化率分别提高了5%和7%。La的加入,抑制了Ni晶粒的团聚,增加了Ni的分散度,与未添加La的催化剂相比非活性碳的生成量减少70%,表现出良好的抗积炭性能。

    Abstract:

    The Ni/Mg/Al catalyst doped with rareearthmetals were prepared by cold plasma decomposition and reduction of hydrotalcite-like compound, and the effects of La and Ce on pyhsico-chemical properties and catalytic performance of dry reforming were studied. The catalysts were characterized by X-ray diffraction (XRD), BET surface area and porosity analysis (BET), X-ray photoelectron spectroscopy and thermogravimetry (TG). The results suggested that hydrotalcite-like precursors were completely decomposed to mesoporous Mg(Ni,Al)O solidsolution which partly reduced to Ni0 by cold plasma jet. The conversion of CO2 and CH4 were 76% and 61.8% at 700 ℃ with V(CH4)/V(CO2)=4/6,GHSV of 30000mL/(h·gcat). The promoter of Ce improved catalyst lattice oxygen concentration and promoted the elimination of carbon species on the catalyst surface,, and the conversion of methane and carbon dioxide were increased by 5% and 7%, respectively. While the promoter of La inhibited the agglomeration of Ni0 and improved the dispersion of Ni0, and the non-active carbon deposition decreased by 70%, showing better anti-coke property.

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龙华丽.等离子体制备稀土金属掺杂甲烷干气重整Ni/Mg/Al催化剂研究[J].精细化工,2017,34(1):

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  • 收稿日期:2016-07-24
  • 最后修改日期:2016-11-11
  • 录用日期:2016-12-07
  • 在线发布日期: 2016-12-30
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