Zr/Al比对Ni-x Zr-Al催化剂在低温联合甲烷蒸汽与干重整反应中性能的影响  

Study of Ni-x Zr-Al catalysts with different Zr/Al ratios for combined methane steam and dry reforming reaction

作　　者：曾文清 李丽 巫学双 宋谋虓 李桂英[2] 胡常伟[1,2] ZENG Wen-qing;LI Li;WU Xue-shuang;SONG Mou-xiao;LI Gui-ying;HU Chang-wei(College of Chemical Engineering,Sichuan University,Chengdu 610065,China;Key Laboratory of Green Chemistry and Technology,Ministry of Education,College of Chemistry,Sichuan University,Chengdu 610064,China)

机构地区：[1]四川大学化学工程学院,四川成都610065 [2]四川大学化学学院绿色化学与技术教育部重点实验室,四川成都610064

出　　处：《化学研究与应用》2022年第10期2398-2407,共10页Chemical Research and Application

基　　金：国家重点研发计划“纤维素类生物质多组分耦合热分解机理及产物定向提质规律”(2018YFB1501404)资助。

摘　　要：由生物质解热尾气转化制备合成气,是促进清洁能源发展的重要途径之一。通过一锅法制备了不同Zr/Al比的10Ni-xZr-Al催化剂,并用于600℃、常压、原料气比例为CH_(4)/CO_(2)/H_(2)O/Ar=1∶0.3∶0.8∶3、总GHSV为15000 mL/(g·h)条件下的联合甲烷蒸汽与干重整反应。结果表明,10Ni-Al无法抑制逆水气变换反应,产生大量积碳,表现出较差的稳定性。而Zr的加入对提高催化稳定性和抑制积碳有一定的促进作用。在Zr/Al比在0.1-0.25时,可以使镍颗粒尺寸保持良好的结构稳定性。其中,10Ni-0.25Zr-Al催化剂在8 h的稳定性实验中,表现出良好的活性及稳定性能(甲烷转化率为50%),获得最低的H_(2)/CO比值为2.5(即最高的CO选择性)。而抗积碳能力最强的是10Ni-0.5Zr-Al催化剂。The preparation of syngas by converting biomass pyrolysis tail gas is one of the important ways to promote the development of clean energy.10Ni- x Zr-Al catalysts with different Zr/Al ratios were prepared by one-pot method and used for combined methane steam and dry reforming reaction at 600℃ under atmospheric pressure,CH_(4)/CO_(2)/H_(2)O/Ar=1∶0.33∶0.8∶3,and a total GHSV of 15000 mL/(g·h).The results showed that 10Ni-Al could not inhibit the inverse water-gas conversion reaction with large amount of carbon accumulated,and then showed poor stability.The addition of Zr has a certain promotion effect on improving the catalytic stability and suppressing the carbon accumulation.At the Zr/Al ratio of 0.1-0.25,good structural stability of nickel particle can be maintained.Among them,the 10Ni-0.25Zr-Al catalyst showed good activity and stable performance(50%methane conversion)in the 8-h stability experiment,and the lowest H_(2)/CO ratio of 2.5(i.e.,the highest CO selectivity)was obtained.The best resistance to carbon build-up was obtained on 10Ni-0.5Zr-Al catalyst.

关 键 词：联合甲烷重整 合成气制备 ZR含量 抗积碳 

分 类 号：O643.3[理学—物理化学]