摘要
采用烷基偶联剂水解法制备(Ni/MgAl_(2)O_(4))@SiO_(2)催化剂,探究Ni、SiO_(2)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(CH_(4)):V(CO_(2)):V(N_(2))=5:5:1、GHSV=26400 mL/(g_(cat)·h)条件下进行DRM反应,(10Ni/MgAl_(2)O_(4))@5SiO_(2)催化剂表现出最好的反应性能,CH_(4)转化率为77%,CO_(2)转化率为90%。通过TEM、SEM等表征发现,SiO_(2)可以包覆在Ni/MgAl_(2)O_(4)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(CH_(4)):V(CO_(2)):V(N_(2))=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/(g_(cat)·h),具有较好的工业应用前景。
A(Ni/MgAl_(2)O_(4))@SiO_(2) catalyst is prepared via alkyl coupling agent hydrolysis method.The influences of Ni loadings and SiO_(2) content on the catalyst's activity and carbon deposition resistance for dry-gas reforming of methane(DRM)are explored.(10Ni/MgAl_(2)O_(4))@5SiO_(2) catalyst shows the best reaction performance when it is applied in DRM reaction under the conditions such as ambient pressure,750℃,v(CH_(4)):v(CO_(2)):v(N_(2))=5:5:1,GHSV=26,400 mL/(g_(cat)·h).The conversion rates of CH_(4) and CO_(2) can reach 77%and 90%,respectively.Through TEM,SEM and other characterizations,it is found that SiO_(2) can coat onto the surface of Ni/MgAl_(2)O_(4) catalyst,hindering the agglomeration of Ni crystal grains and increasing the resistance to carbon deposition.The(10Ni/MgAl_(2)O_(4))@5SiO_(2) catalyst is subjected to a 450 h stability test under severe conditions of v(CH_(4)):v(CO_(2)):v(N_(2))=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/(g_(cat)·h),representing a potential application in industry.
作者
苗晓玲
吴东
沈卫华
王俊有
高鑫华
方云进
MIAO Xiao-ling;WU Dong;SHEN Wei-hua;WANG Jun-you;GAO Xin-hua;FANG Yun-jin(State Key Laboratory of Chemical Engineering,East China University of Science and Technology,Shanghai 200237,China)
出处
《现代化工》
CAS
CSCD
北大核心
2022年第3期98-103,108,共7页
Modern Chemical Industry
基金
国家自然科学基金(21576083)。
关键词
干气重整
核壳型
尖晶石
抗积碳
dry gas reforming
core-shell type
spinel
resistance to carbon deposition
