等离子体辅助制备低温高活性CO_(2)催化还原用Y_(2)O_(3)-Ni/CeO_(2)催化剂  

Plasma-assisted preparation of Y_(2)O_(3)-Ni/CeO_(2) catalyst with low temperature and high activity for catalytic reduction of CO_(2)

作　　者：梅加 马军 肖鑫[1] 李露明 高新华[3] 储伟[1] MEI Jia;MA Jun;XIAO Xin;LI Luming;GAO Xinhua;CHU Wei(School of Chemical Engineering,Sichuan University,Chengdu 610065,Sichuan,China;Institute for Advanced Study,Chengdu University,Chengdu 610106,Sichuan,China;State Key Laboratory of High-Efficiency Utilization of Coal and Green Chemical Engineering,Ningxia University,Yinchuan 750021,Ningxia,China)

机构地区：[1]四川大学化学工程学院,四川成都610065 [2]成都大学高等研究院,四川成都610106 [3]宁夏大学省部共建煤炭高效利用与绿色化工国家重点实验室,宁夏银川750021

出　　处：《天然气化工—C1化学与化工》2022年第4期25-31,共7页Natural Gas Chemical Industry

摘　　要：以CeO_(2)为载体,采用浸渍法和N2辉光等离子体辅助处理制备了一系列不同含量(质量分数,下同)的Y_(2)O_(3)促进的Ni/CeO_(2)催化剂,研究了该处理方法下Y_(2)O_(3)含量对催化剂结构和低温反应性能的影响。结果表明,在CO_(2)催化还原制合成天然气反应中,随着Y_(2)O_(3)含量的增加,Y_(2)O_(3)-Ni/CeO_(2)的反应活性先升高后降低。在220℃,n(H_(2)):n(CO_(2))=4:1,空速15000 mL/(g·h)时,1.5Y_(2)O_(3)-Ni/CeO_(2)表现出最优异的低温催化反应活性,CO_(2)转化率达到84.1%,CH_(4)选择性为100%。Y_(2)O_(3)的加入增强了活性组分Ni的分散度和还原度,增加了催化剂表面活性位数量,并调控了催化剂上的碱性位和氧空位含量,提高了低温下的反应活性。对1.5Y_(2)O_(3)-Ni/CeO_(2)进行80 h稳定性测试,发现CO_(2)转化率始终维持在85.0%左右,CH_(4)选择性为100%。A series of Ni/CeO_(2) catalysts promoted by different contents(mass fraction,the same below)of Y_(2)O_(3) were prepared by impregnation and N_(2) glow plasma-assisted treatment method with CeO_(2) as carrier.The effects of the contents of Y_(2)O_(3) on the structure and the low-temperature reaction performance of the catalysts were studied.The results show that the catalytic activity of Y_(2)O_(3)-Ni/CeO_(2) catalysts improves first and then decreases with the increase of Y_(2)O_(3) content in the CO_(2) catalytic reduction to synthetic natural gas reaction.Under the reaction conditions of 220℃,n(H_(2)):n(CO_(2))=4:1 and space velocity 15000 mL/(g·h),1.5Y_(2)O_(3)-Ni/CeO_(2) catalysts show the most excellent low-temperature catalytic activity with CO_(2) conversion of 84.1%and CH_(4) selectivity of 100%.The addition of Y_(2)O_(3) enhances the dispersion and reducibility of the active component Ni,and increases the active sites on the catalyst surface,and regulates the content of alkaline sites and oxygen vacancy concentration on the catalyst,and improves the reaction activity at low temperature.The 80 h stability test of 1.5Y_(2)O_(3)-Ni/CeO_(2) catalyst shows that the CO_(2) conversion is maintained at about 85.0%and the CH_(4) selectivity is 100%.

关 键 词：CO_(2)催化还原 等离子体 NI基催化剂 Y2O_(3) 合成天然气 

分 类 号：TQ209[化学工程—有机化工] O643.3[理学—物理化学]