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摘要
采用烷基偶联剂水解法制备(Ni/MgAl2O4)@SiO2催化剂,探究Ni、SiO2质量分数对催化剂的甲烷干气重整(DRM)反应活性和抗积碳性能的影响。在常压、750℃、V(CH4):V(CO2):V(N2)=5:5:1、GHSV=26 400 mL/(gcat·h)条件下进行DRM反应,(10Ni/MgAl2O4)@5SiO2催化剂表现出最好的反应性能,CH4转化率为77%,CO2转化率为90%。通过TEM、SEM等表征发现,SiO2可以包覆在Ni/MgAl2O4催化剂表面,阻碍Ni晶粒团聚,增大催化剂的抗积碳性能。将该催化剂在严苛条件[V(CH4):V(CO2):V(N2)=8:2:1]下进行450 h稳定性测试,结果发现催化剂反应活性稳定,平均积碳速率仅为0.10 mg/(gcat·h),具有较好的工业应用前景。
Abstract
A (Ni/MgAl2O4)@SiO2 catalyst is prepared via alkyl coupling agent hydrolysis method.The influences of Ni loadings and SiO2 content on the catalyst's activity and carbon deposition resistance for dry-gas reforming of methane (DRM) are explored.(10Ni/MgAl2O4)@5SiO2 catalyst shows the best reaction performance when it is applied in DRM reaction under the conditions such as ambient pressure,750℃,v(CH4):v(CO2):v(N2)=5:5:1,GHSV=26,400 mL/(gcat·h).The conversion rates of CH4 and CO2 can reach 77% and 90%,respectively.Through TEM,SEM and other characterizations,it is found that SiO2 can coat onto the surface of Ni/MgAl2O4 catalyst,hindering the agglomeration of Ni crystal grains and increasing the resistance to carbon deposition.The (10Ni/MgAl2O4)@5SiO2 catalyst is subjected to a 450 h stability test under severe conditions of v(CH4):v(CO2):v(N2)=8:2:1.It is found that the reaction activity of the catalyst remains stable and the structure after the reaction is still complete.The average carbon deposition rate is as low as 0.10 mg/(gcat·h),representing a potential application in industry.
关键词
干气重整
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抗积碳
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尖晶石
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核壳型
Key words
dry gas reforming
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resistance to carbon deposition
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spinel
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core-shell type
Author summay
苗晓玲(1996-),女,硕士研究生,研究方向为甲烷重整,18443102009@163.com;沈卫华(1977-),男,博士,副教授,研究方向为绿色化工及催化工程,通讯联系人,whshen@ecust.edu.cn。
甲烷干气重整(Ni/MgAl2O4)@SiO2催化剂的制备及抗积碳性能研究[J].
, 2022, 42(3): 98-103,108 DOI:10.16606/j.cnki.issn0253-4320.2022.03.020