LaAl_(0.5)Ni_(0.5)O_(3)钙钛矿的制备及其对甲烷干重整的催化性能  

The Preparation of LaAl_(0.5)Ni_(0.5)O_(3) Perovskite and Its Catalytic Performance in Methane Dry Reforming

作　　者：马于杰 葛以赵 苏鹏 王自军[1] 李永生[2] MA Yujie;GE Yizhao;SU Peng;WANG Zijun;LI Yongsheng(School of Chemistry and Chemical Engineering, Shihezi University/The Xinjiang Production and Construction Corps Key Laboratory for Green Processing of Chemistry and Chemical Engineering,Shihezi 832003, China;School of Materials Science and Engineering, East China University of Science and Technology/MOE Key Laboratory for Ultrafine Materials, Shanghai 200237, China)

机构地区：[1]石河子大学化学化工学院/新疆兵团绿色化学重点实验室,石河子832003 [2]华东理工大学材料科学与工程学院/超细材料制备与应用教育部重点实验室,上海200237

出　　处：《华南师范大学学报（自然科学版）》2022年第3期53-61,共9页Journal of South China Normal University(Natural Science Edition)

基　　金：国家自然科学基金项目(21566031,21766029)。

摘　　要：采用硬模板法制备比表面积大的介孔LaAl_(1-x)Ni_(x)O_(3)钙钛矿催化剂,将其用于碳中和甲烷干重整领域,研究不同温度下的反应活性。通过扫描电子显微镜(SEM)、透射电子显微镜(TEM)、X射线衍射仪(XRD)、N_(2)吸附-脱附(BET)、H_(2)程序升温还原(H_(2)-TPR)、热重分析(TGA)对制备的催化剂进行表征。结果表明:LaAl_(0.5)Ni_(0.5)O_(3)催化剂在反应过程中表现出了最优异的活性与稳定性。在反应温度为750℃,空速GHSV=36000 mL/(g·h)的反应条件下,CH_(4)与CO_(2)的转化率分别达到69.8%和81.5%,经25 h稳定性测试后CH_(4)与CO_(2)的转化率仅分别降低2.7%和3.3%。这是由于在H_(2)-Ar混合气还原过程中,LaAl_(0.5)Ni_(0.5)O_(3)催化剂获得了比LaAl_(0.7)Ni_(0.3)O_(3)催化剂更多的Ni活性位点,同时获得了比LaAl_(0.3)Ni_(0.7)O_(3)催化剂更优异的抗烧结、抗积碳性能。The hard template method was used to prepare the mesoporous LaAl_(1-x)Al_(x)O_(3) perovskite catalyst with a large surface area,which was used for carbon-neutral methane dry reforming for reaction activity test at different temperatures.With scanning electron microscope(SEM),transmission electron microscope(TEM),X-ray diffractometer(XRD),N_(2) adsorption and desorption(BET),H_(2) temperature programmed reduction(H_(2)-TPR),thermogravimetric analysis(TGA)and other methods,the as-prepared catalyst was characterized.The results showed that the LaAl_(0.3)Ni_(0.7)O_(3) catalyst exhibited the most excellent activity and stability during the reaction,the initial activity of CH_(4) and CO_(2) in the LaAl_(0.3)Ni_(0.7)O_(3) catalyst reached 69.8%and 81.5%respectively under the conditions of reaction temperature of 750℃and space velocity GHSV=36000 mL/(g·h).And the CH_(4) and CO_(2) activity of the LaAl_(0.3)Ni_(0.7)O_(3) catalyst reduced by 2.7%and 3.3%respectively after the 25 h stability test.The reason was that the LaAl_(0.3)Ni_(0.7)O_(3) catalyst obtained more Ni active sites than the LaAl_(0.7)Ni_(0.3)O_(3) catalyst and the LaAl_(0.3)Ni_(0.7)O_(3) catalyst had more favorable anti-sintering and anti-carbon deposition ability than the LaAl0.3Ni0.7O3 catalyst.

关 键 词：硬模板法 碳中和 Ni基钙钛矿 甲烷干重整 

分 类 号：O643.3[理学—物理化学]