摘要
采用并流共沉淀法制备了不同镓锆比(Ga/Zr=2/8、3/7、4/6、5/5)的Ga_(y)Zr_(1-y)O_(x)(y=0.2、0.3、0.4、0.5)催化剂,探究Ga掺杂比例对催化剂性能的影响,获得最佳的Ga/Zr比例。通过XRD、N_(2)物理吸附、ICP-OES和TG等表征手段分别对Ga_(y)Zr_(1-y)O_(x)催化剂的材料的晶相、比表面积、孔容、孔径和失重等参数进行研究;通过XPS、CO_(2)-TPD、H_(2)-TPD和H_(2)-TPR考察材料表面电子结构、酸碱性、还原性和H_(2)及CO_(2)吸附性等,揭示材料结构与性能之间的关系。实验表明随着Ga掺杂比例增大,Ga_(y)Zr_(1-y)O_(x)催化剂的比表面积和分散度显著提高,H_(2)/CO_(2)吸附量和中等碱性位点数量显著增加,表面氧空位含量增多以及Ga与Zr相互作用增强。适宜的Ga含量有利于提高Ga_(y)Zr_(1-y)O_(x)催化剂的催化性能,当Ga/Zr=4/6时,在280℃、3 MPa、H_(2)/CO_(2)=3/1的条件下,甲醇时空产率最高达到4.95 mmol/h·gcat。
A series of Ga_(y)Zr_(1-y)O_(x)(y=0.2,0.3,0.4,0.5)catalysts with different Ga-Zr ratios(Ga/Zr=2/8,3/7,4/6,5/5)were prepared by co-current coprecipitation method.The effect of Ga doping ratio on catalyst performance was investigated,and the optimal Ga/Zr ratio was obtained.The crystal phase,specific surface area,pore volume,pore size and weight loss of Ga_(y)Zr_(1-y)O_(x)catalyst materials were studied by XRD,N_(2)physical adsorption,ICP-OES and TG.XPS,CO_(2)-TPD,H_(2)-TPD and H_(2)-TPR were used to investigate the surface electronic structure,acid-alkalinity,reducibility and H_(2)and CO_(2)adsorbability of the materials,and to reveal the relationship between the structure and properties of the materials.The results show that the specific surface area and dispersion of Ga_(y)Zr_(1-y)O_(x)catalyst increase significantly with the increase of Ga doping ratio.The adsorption capacity of H_(2)/CO_(2)and the number of moderately alkaline sites increased significantly.The surface oxygen vacancy content increases and the interaction between Ga and Zr is enhanced.Appropriate Ga content can improve the catalytic performance of Ga_(y)Zr_(1-y)O_(x)catalyst.When Ga/Zr=4/6,at the condition of 280℃,3 MPa,H_(2)/CO_(2)=3/1,the maximum methanol yield reached 4.95 mmol/(h·g cat).
作者
陈志远
周嘉宾
黄振辉
王宇宁
龚杰松
高文桂
CHEN Zhiyuan;ZHOU Jiabin;HUANG Zhenhui;WANG Yuning;GONG Jiesong;GAO Wengui(School of Metallurgical and Energy Engineering,Kunming University of Science and Technology,Kunming 650093,China;State Key Laboratory of Clean Utilization of Complex Non-Ferrous Metal Resources,Kunming University of Science and Technology,Kunming 650093,China)
出处
《功能材料》
CAS
CSCD
北大核心
2024年第12期12175-12184,共10页
Journal of Functional Materials
基金
云南省科技厅科技计划(202302AG050005-2)
云南省万人计划(YNWR-QNBJ-2020-016)。
关键词
CO_(2)加氢
甲醇
并流共沉淀法
掺杂比例
改性研究
CO_(2)hydrogenation
methanol
co-current coprecipitation method
doping ratio
modification study
作者简介
通讯作者:高文桂,E-mail:gao_wengui@126.com;陈志远(1998-),男,硕士研究生,师承高文桂教授,主要从事节能减排和CO_(2)资源化利用研究。
