Mg修饰Fe/Al载氧体煤化学链制氢  

Chemical looping hydrogen generation of coal with oxygen carrier of Mg-modified Fe/Al

作　　者：安阳 袁思杰 高振东 吴曼[1] 王凌云 郭庆杰[1] AN Yang;YUAN Sijie;GAO Zhendong;WU Man;WANG Lingyun;GUO Qingjie(College of Chemical Engineering,Qingdao University of Science and Technology,Qingdao 266042,Shandong,China)

机构地区：[1]青岛科技大学化工学院,山东青岛266042

出　　处：《化工进展》2022年第2期648-654,共7页Chemical Industry and Engineering Progress

基　　金：国家自然科学基金联合基金重点项目(U20A20124);国家重点研发计划(2018YFB0605401);宁夏回族自治区重点研发计划(重大科技)项目(2018BCE01002);国家自然科学基金地区项目(21868025);宁夏高等学校一流学科建设项目(NXYLXK2017A04)。

摘　　要：目前化学链过程常用的Fe_(2)O_(3)/Al_(2)O_(3)载氧体会形成FeAl_(2)O_(4),因热力学限制很难与水反应制氢。为了抑制FeAl_(2)O_(4)的形成,本文向Fe/Al载氧体中添加Mg,在固定床上进行煤化学链制氢(CLHG),深入分析Mg的作用机理并探究其对实验结果的影响。XRD结果表明,Mg质量分数从1%增加到26.5%时,MgAl_(2)O_(4)特征峰增强,FeAl_(2)O_(4)特征峰逐渐消失,说明Mg减弱了Fe和Al之间的相互作用。SEM显示Mg添加后载氧体颗粒减小,耐烧结性能优异。对比不同煤/载氧体质量比的实验,质量比为0.5/15时碳转化率和产氢量最高。在不同Mg含量的载氧体中,Fe40Mg20Al40具备最好的反应性能,碳转化率和产氢量为81.75%和1.7182L/g,比Fe40Al60分别增加10.2%和58.5%。Fe40Mg20Al40经10次循环,表面仅有轻微烧结,碳转化率和产氢量均在78%和1.52L/g以上,循环性能良好。添加Mg可以有效抑制FeAl_(2)O_(4)的生成,显著增强蒸汽氧化过程的反应活性,大幅提高氢气产量,十分适用于煤化学链制氢。Fe_(2)O_(3)/Al_(2)O_(3) oxygen carrier used in chemical looping process will form FeAl_(2)O_(4),which is difficult to react with water to produce hydrogen due to thermodynamic limitations.In order to solve this problem,Mg was added to Fe/Al oxygen carrier for coal chemical looping hydrogen generation,and the action mechanism of Mg was deeply analyzed and its influence on the experimental results was explored.The XRD results show that when the Mg content increases from 1%to 26.5%,the characteristic peak of MgAl_(2)O_(4) increases,and the characteristic peak of FeAl_(2)O_(4) gradually disappears,indicating that Mg weakens the interaction between Fe and Al.SEM shows that the size of oxygen carrier particles decrease after adding Mg,and the sintering resistance is excellent.Based on the experiments of different coal/oxygen-carrier mass ratio,the carbon conversion and hydrogen production were the highest when the mass ratio was 0.5/15.Among the oxygen carriers with different Mg contents,Fe40Mg20Al40 has the best reaction performance,and the carbon conversion and hydrogen production are 81.75%and 1.7182L/g,which increase by 10.2%and 58.5%compared with Fe40Al60,respectively.After 10 cycles,the surface of Fe40Mg20Al40 is only slightly sintered,and the carbon conversion and hydrogen production are above 78%and 1.52L/g,respectively,showing good cycling performance.The addition of Mg can effectively inhibit the formation of FeAl_(2)O_(4),significantly enhance the reactivity of steam oxidation process,and greatly increase the yield of hydrogen,which is very suitable for coal chemical looping hydrogen generation.

关 键 词：Fe基载氧体 FeAl_(2)O_(4) MgAl_(2)O_(4) 化学链制氢 煤 

分 类 号：TQ116.2[化学工程—无机化工]