首页|Mg-Al-hydrotalcite with alkaline sites protects Ni/KIT-6 from formation of amorphous coke in glycerol steam reforming via tailoring reaction intermediates
Mg-Al-hydrotalcite with alkaline sites protects Ni/KIT-6 from formation of amorphous coke in glycerol steam reforming via tailoring reaction intermediates
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During steam reforming,the performance of a catalyst and amount/property of coke are closely related to reaction intermediates reaching surface of a catalyst.Herein,modification of reaction intermediates by placing Mg-Al-hydrotalcite above Ni/KIT-6 catalyst in steam reforming of glycerol was conducted at 300 to 600 ℃.The results revealed that the catalytic activity of Ni/KIT-6 in the lower bed was enhanced with either Mg1-Al5-hydrotalcite(containing more acidic sites)or Mg5-Al1-hydrotalcite(containing more alkaline sites)as upper-layer catalyst.The in situ infrared characterization of steam reforming demonstrated that Mg-Al-hydrotalcite catalyzed the deoxygenation of glycerol,facilitating the reforming of the partially deoxygenated intermediates over Ni/KIT-6.Mg-Al-hydrotalcite as protective catalyst,however,did not protect the Ni/KIT-6 from formation of more coke.Nonetheless,this did not lead to further deactivation of Ni/KIT-6 while Mg5-Al1-hydrotalcite even substantially enhanced the catalytic stability,even though the coke was much more significant than that in the use of single Ni/KIT-6(52.7％ vs.28.6％).The reason beneath this was change of the property of coke from more aliphatic to more aromatic.Mg5-Al1-hydrotalcite catalyzed dehydra-tion of glycerol,producing dominantly reaction interme-diates bearing C=C,which formed the catalytic coke of with carbon nanotube as the main form with smooth outer walls as well as higher aromaticity,C/H ratio,crystallinity,crystal carbon size,thermal stability,and resistivity toward oxidation on Ni/KIT-6 in the lower bed.In comparison,the abundance of acidic sites on Mg1-Al5-hydrotalcite catalyzed the formation of more oxygen-containing species,leading to the formation of carbon nanotubes of rough surface on Ni/KIT-6.
steam reforming of glycerolMg-Al-hydrotalcitesacrificial catalystreaction intermediatesproperty of coke
Yunyu Guo、Yiran Wang、Yuewen Shao、Shu Zhang、Yi Wang、Song Hu、Jun Xiang、Xun Hu
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School of Material Science and Engineering,University of Jinan,Jinan 250022,China
Joint International Research Laboratory of Biomass Energy and Materials,College of Materials Science and Engineering,Nanjing Forestry University,Nanjing 210037,China
State Key Laboratory of Coal Combustion,Huazhong University of Science and Technology,Wuhan 430074,China
国家自然科学基金Program for Supporting Innovative Research of JinanProgram for Agricultural Development of Shandong
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