Co-Cu-M(M=Fe,Mn,Ni,Zn,Ce)催化剂催化分解N_2O性能
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摘要
采用等体积浸渍法制备了添加不同金属助剂的铜钴复合氧化物(Co/Cu质量比为0.6)催化剂,考察了其催化N_2O分解的活性。结果表明,稀土金属Ce以及过渡金属Fe对钴铜催化剂催化N_2O分解的活性有明显的促进作用。通过分析催化剂的X射线衍射(XRD)、比表面积测定(BET)、氢气程序升温还原(H_2-TPR)以及扫描电镜(SEM)等表征结果发现,助剂的添加并没有引起催化剂晶相结构的明显改变,但可以提高钴离子与铜离子的还原能力。尤其是添加Ce和Fe之后还原峰向低温区显著移动,从而提高了钴铜复合氧化物催化剂的活性。
Catalysts of Co-Cu composite oxides doped with metals cocatalysts were prepared using the impregnation method and their activity in the catalytic decomposition of N_2 O were tested. The results showed that the catalytic activity of Co-Cu composite oxide was largely enhanced by the addition of rare earth Ce and transition metal Fe. XRD,BET,SEM,and H_2-TPR were used to characterize the Cu-Co composite oxide catalysts,and the results showed that the addition of the cocatalyst did not change the catalysts' crystal structures,but did enhance the reduction ability of the Co and Cu ions. The reduction peaks even shifted to the low temperature region after adding Ce and Fe,and therefore the catalytic activity for the decomposition of N_2 O was improved.
Catalysts of Co-Cu composite oxides doped with metals cocatalysts were prepared using the impregnation method and their activity in the catalytic decomposition of N_2 O were tested. The results showed that the catalytic activity of Co-Cu composite oxide was largely enhanced by the addition of rare earth Ce and transition metal Fe. XRD,BET,SEM,and H_2-TPR were used to characterize the Cu-Co composite oxide catalysts,and the results showed that the addition of the cocatalyst did not change the catalysts' crystal structures,but did enhance the reduction ability of the Co and Cu ions. The reduction peaks even shifted to the low temperature region after adding Ce and Fe,and therefore the catalytic activity for the decomposition of N_2 O was improved.
引文
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[18]张海杰,王建,窦喆,等.Cu-Co-Al复合氧化物在N2O分解反应中的催化活性[J].石油化工,2015,44(2):235-240.
[2]中国气象局.2013年中国温室气体公报[EB/OL].2015-01-09.http://www.cma.gov.cn/2011xwzx/2011xqxxw/2011xqxyw/201501/t20150109_271700.html.
[3]林峰,黎维彬,杨良针.负载Mn-Co复合氧化物的椰炭对氮氧化物的吸附[J].化工环保,2011,31(5):455-458.
[4]联合国环境规划署.世界环境数据手册[M].北京:中国科学技术出版社,1990:19-20.
[5]周浩生,陆继东,周琥,等.流化床燃煤过程降低N2O排放措施评述[J].热能动力工程,2000,15(1):1-3.
[6]李宁.N2O分解催化剂的制备[J].化工进展,2007,26(11):1659-1661.
[7]STEFANO A,FRANCESCON B,SONIA B,et al.Development of new catalysts for N2O decomposition from adipicacdpant[J].Appl.Catal.B:Environ.,2007,70:323-329.
[8]THIEMENS M H,WILLIAM C T.Nylon production:an unknown dource of atmospheric nitrous oxide[J].Science,1991,251:932-934.
[9]OBALOVáL,FILA V.Kinetic analysis of N2O decomosition over calcined hydrotalcites[J].Appl.Catal.B,2007,70(1/4):353-359.
[10]CHENG H,HUANG Y,WANG A,et al.N2O decompositinover K-promted Co-Al catalysts prepared from hydrotalcite-like precursors[J].Appl.Catal.B,2009,89(3/4):391-397.
[11]周涛,刘少光,唐明早,等.选择性催化还原脱硝催化剂研究进展[J].硅酸盐学报,2009,37(2):317-324.
[12]HANS BEYER,JENS Emmerichl,KONSTANTINOS Chatziapostolou,et al.Decomposition of nitro-us oxide by rhodiumcatalysts:effect of rhodium particle sizea and metal oxide support[J].Applied Catalysis A:General,2011,39(1):411-416.
[13]胡云峰,潘志强,刘万成,等.共沉淀法制备Cu/Zn O催化剂用于1,4-丁二醇合成吡咯[J].化工进展,2014,33(4):941-946.
[14]XUE Li,ZHANG Chongbin,HE Hong,et al.Catalytic decom-position of N2O over Ce O2 promoted Co3O4 spinel catalyst[J].Appl.Catal.B,2007,75(3/4):167-174.
[15]徐秀峰,索掌怀,魏玉萍,等.Cu、Co交换改性蒙脱土的制备及其对N2O分解的催化活性[J].燃料化学学,2001,29(3):247-250.
[16]赵晓旭,程党国,陈丰秋,等.N2O直接分解催化剂的研究进展[J].化工进展,2009,28(9):1562-1567.
[17]宋永吉,李翠清,董留涛,等.铜锌掺杂的六铝酸盐分解N2O催化性能研究[J].工业催化,2008,16(10):172-175.
[18]张海杰,王建,窦喆,等.Cu-Co-Al复合氧化物在N2O分解反应中的催化活性[J].石油化工,2015,44(2):235-240.