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作 者:颜再荣 苗超 刘庆贺[1,2] 韩菲 欧阳静[1,2,3] YAN Zai Rong;MIAO Chao;LIU Qing He;HAN Fei;OU YANG Jing(Hunan Key Lab of Mineral Materials and Application,Central South University,Changsha 410083,China;Centre for Mineral Materials,Department of Inorganic Materials,School of Resources and Bioengineering,Central South University,Changsha 410083,China;Key Lab of Clay Mineral Functional Materials in China Building Materials Industry,Central South University,Changsha 410083,China)
机构地区:[1]中南大学湖南省矿物材料与应用重点实验室,长沙410083 [2]中南大学资源与生物工程学院无机材料系矿物材料中心,长沙410083 [3]中国建筑材料行业创新平台黏土矿物功能材料重点实验室,长沙410083
出 处:《硅酸盐学报》2021年第7期1377-1384,共8页Journal of The Chinese Ceramic Society
基 金:国家自然科学基金(51774331);中南大学研究生自主创新项目(1053320183283)资助。
摘 要:基于黏土矿物在催化剂制品中的广泛应用和因CO_(2)增长过快造成的全球温室效应,通过溶胶凝胶法在凹凸棒石(ATP)表面负载TiO_(2)并以其为载体,采用浸渍法制备了用于CO_(2)甲烷化的Ni-Ru/TiO_(2)-ATP催化剂。比较Ru和Ni负载量对催化性能的影响,重点考察了反应温度和空速对甲烷化过程的影响,并采用原位红外测试技术进一步揭示了其反应机理。结果表明:双金属催化剂具有优异的低温催化活性。制备的催化剂中5Ni-1Ru-TiO_(2)-ATP的催化效果最佳,在350℃时CO_(2)转化率达到47.9%,在400℃时转化率最高,为59.6%。比相同条件下制备的不含Ru的催化剂在350℃时的转化率提高31.8%,在400℃时提高26.5%。进气速率过大会导致气固相接触不充分,催化效果变差。原位红外分析发现该多元复合催化剂遵循一种以CO~*基团为中间体的反应机理。Noting the extensive application of minerals in catalysts and the urgent solution to address the global greenhouse problem caused by the too fast release of CO_(2),TiO_(2)-attapulgite(ATP)was prepared by using a sol-gel method,on which Ni-Ru catalyst was loaded through impregnation for CO_(2) methanation.Performances of the samples with different contents of Ru and Ni were compared,while the influence of CO_(2) intake rate was especially studied and the reaction mechanism was explored by using in-situ IR spectroscopy.It was found that the bimetallic catalyst had excellent low temperature activities,whereas the effect of Ru was more pronounced.Among the catalysts prepared,5Ni-1Ru-TiO_(2)-ATP has the best catalytic effect,with the CO_(2) conversion rate reaching 47.9%at 350℃and the highest(59.6%)at 400℃.Compared with the catalyst without Ru prepared under the same conditions,the conversion rate at 350℃was increased by 31.8%,and at 400℃by 26.5%.Excessive intake rate leads to insufficient gas-solid contact and poor catalytic effect.The composite catalyst followed a reaction path with CO*radicals as the intermediate.
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