Ni-xFe/Mayenite促进CO_(2)-CH_(4)重整的稳定性调控实验研究  

Experimental Investigations on Stability Tailoring of Ni-xFe/Mayenite for CO_(2)-CH4 Reforming

作　　者：陈玉民[1] 卢钱程 任燕燕 彭瑞峰 张兵[1] 黄文捷 赵永椿[2] 张军营[2] Chen Yumin;Lu Qiancheng;Ren Yanyan;Peng Ruifeng;Zhang Bing;Huang Wenjie;Zhao Yongchun;Zhang Junying(School of Low Carbon Energy and Power Engineering,China University of Mining and Technology,Xuzhou 221116,China;State Key Laboratory of Coal Combustion,Huazhong University of Science and Technology,Wuhan 430074,China)

机构地区：[1]中国矿业大学低碳能源与动力工程学院,徐州221116 [2]华中科技大学煤燃烧国家重点实验室,武汉430074

出　　处：《燃烧科学与技术》2022年第3期229-238,共10页Journal of Combustion Science and Technology

基　　金：中央高校基本科研业务费专项资金资助项目(2020ZDPYMS23);国家重点研发计划资助项目(2017YFB0601900).

摘　　要：采用湿法混合-浸渍法制备了一系列Ni-xFe/mayenite(Ca_(12)Al_(14)O_(33))催化剂,并在700℃、常压、CH_(4)/CO_(2)为1的条件下进行了干重整实验研究.系统考察了金属负载量、金属组分等对干重整活性和稳定性的影响.其中7.5%Ni-0.1Fe/mayenite能够得到接近热力学平衡值的CO_(2)和CH_(4)转化率(分别为90.1%、86.0%),氢碳比为0.94.Ni-xFe/mayenite的活性随着Ni负载量从5%增加到10%显著提高;进一步增加到30%时,活性提升有限.Ni负载量较高的Ni/mayenite更容易发生碳沉积,导致反应器堵塞,而Ni-xFe/mayenite在干重整过程中稳定性显著提高.Fe掺杂提高催化剂表面氧浓度,形成Ni-Fe合金有利于Ni位点分散,抑制CH_(4)过快裂解;钙铝石作为载体,促进了CO_(2)与金属之间的氧传递效率,提高了Ni表面的积碳氧化速率.A series of Ni-xFe/mayenite(Ca_(12)Al_(14)O_(33))catalysts were prepared by co-impregnation method,and tested for dry reforming(DRM)at 700℃,atmospheric pressure and a feeding CH_(4)/CO_(2)ratio of 1.Effects of metal loading and metal composition on DRM activity and stability of Ni-xFe/mayenite were systematically investigated.The 7.5%Ni-0.1Fe/mayenite catalyst achieved a CO_(2)and CH_(4)conversion rate(90.1%and 86.0%,respectively),approximate to the thermodynamic equilibrium values,and the H_(2)/CO ratio was 0.94.With mayenite as support,the activity of Ni-xFe/mayenite catalysts improved greatly as Ni content increased from 5%to 10%,whereas lim-ited increase of activity was observed when Ni content further increased to 30%.Ni/mayenite with higher metal loading was more prone to carbon disposition,leading to reactor blockage,while Ni-xFe/mayenite showed much better stability during DRM.Fe doping would increase surface oxygen concentration and enhance the dispersion of nickel sites,hence preventing the over-fast dissociation of CH_(4).Mayenite as support was supposed to enhance the oxygen transfer from CO_(2)to the active metal,thus promote the oxidation of coke depositing on Ni surface.

关 键 词：干重整 钙铝石 镍-铁 抗积碳 

分 类 号：TK11[动力工程及工程热物理—热能工程]