正丁烷在Au,Zn组合改性纳米HZSM-5上的催化转化

催化学报 , 2013, 34(6): 1262-1266. doi: 10.1016/S1872-2067(12)60539-7

正丁烷在Au,Zn组合改性纳米HZSM-5上的催化转化

艾沙·努拉洪 ^1, , 刘家旭 ^2, , 贺宁 ^3, , 郭洪臣 ^4,

1.大连理工大学化工学院催化化学与工程系精细化工国家重点实验室,辽宁大连116024

2.大连理工大学化工学院催化化学与工程系精细化工国家重点实验室,辽宁大连116024

3.大连理工大学化工学院催化化学与工程系精细化工国家重点实验室,辽宁大连116024

4.大连理工大学化工学院催化化学与工程系精细化工国家重点实验室,辽宁大连116024

关键词：金 , 锌 , HZSM-5分子筛 , 正丁烷转化 , 脱氢 , 芳构化 , 纳米金颗粒 , 沉积沉淀法

Catalytic conversion of n-butane over Au-Zn-modified nano-sized HZSM-5

AI SHA·Nu La Hong ^1, , LIU Jiaxu ^2, , HE Ning ^3, , GUO Hongchen ^4,

1.大连理工大学化工学院催化化学与工程系精细化工国家重点实验室,辽宁大连116024

2.大连理工大学化工学院催化化学与工程系精细化工国家重点实验室,辽宁大连116024

3.大连理工大学化工学院催化化学与工程系精细化工国家重点实验室,辽宁大连116024

4.大连理工大学化工学院催化化学与工程系精细化工国家重点实验室,辽宁大连116024

Keywords： Gold , Zinc , HZSM-5 zeolite , n-Butane conversion , Dehydrogenation , Aromatization , Nano-gold particle , Deposition-precipitation

采用沉积沉淀和浸渍法制备了Au-Zn组合改性HZSM-5催化剂.并且对比研究了HZSM-5,Au/HZSM-5,Zn/HZSM-5和Au-Zn/HZSM-5催化剂的性质和催化性能.采用UV-Vis和XPS表征揭示出Au-Zn/HZSM-5催化剂中Au物种与Zn物种的相互作用.正丁烷探针反应结果表明,在Zn/HZSM-5催化剂中引入Au有效地提高了正丁烷的脱氢芳构化性能,同时抑制了正丁烷在Zn活性中心上的氢解副反应.在相同条件下,与Zn/HZSM-5催化剂相比,正丁烷转化率由49.1％增加到70.8％,烯烃和芳烃产物总选择性由57％增加到61.98％,干气的选择性由31％降低至28.4％.上述结果表明,Au-Zn/HZSM-5催化剂在轻烃芳构化反应中具有良好的催化性能.

参考文献

[1]	Cheung TK.;Gates BC.;Ditri JL. .CRACKING OF N-BUTANE CATALYZED BY IRON- AND MANGANESE-PROMOTED SULFATED ZIRCONIA[J].Journal of Catalysis,1995(2):344-349.
[2]	Bedell M W;Ruszica P A;Steffens T R.[J].Presentation at the 2003 Tulane Engineering Forum,2003
[3]	Park Y K;Lee C W;Kang N Y;Choi C W Choi S Oh S H Park D S .[J].CATALYSIS SURVEYS FROM ASIA,2010,14:75.
[4]	Zhang J;Liu X;Blume R;Zhang A H Schlogl R Su D S .[J].SCIENCE,2008,322(5898):73.
[5]	Huff M;Schmidt L D .[J].Journal of Catalysis,1994,149:127.
[6]	Ge S H;Liu C H;Zhang S C;Li Z H .[J].CHEMICAL ENGINEERING JOURNAL,2003,94:121.
[7]	Lu J Y;Zhao Z;Xu C M;Zhang P Duan A J .[J].CATALYSIS COMMUNICATIONS,2006,7:199.
[8]	Lu, JY;Zhao, Z;Xu, CM;Duan, AJ;Zhang, P .CrHZSM-5 zeolites - Highly efficient catalysts for catalytic cracking of isobutane to produce light olefins[J].Catalysis Letters,2006(1/2):65-70.
[9]	Jiang G Y;Zhang L;Zhao Z;Zhou X Y Duan A J Xu C M Gao J S .[J].Applied Catalysis A:General,2008,340:176.
[10]	Rahimi N;Karimzadeh R .[J].Applied Catalysis A:General,2011,398:1.
[11]	Ono Y;Kanae K;J Chem Soc .[J].Fraday Trans,1991,87:663.
[12]	OnoY .[J].CatalRev-SciEng,1992,34:179.
[13]	Caeiro G;Carvalho R H;Wang X;Lemos M A N D A Lemos F Guisnet M Ribeiro F R .[J].Journal of Molecular Catalysis A:Chemical,2006,255:131.
[14]	Xu Y B;Ma H T;Yamamoto Y;Suzuki Y Zhang Z G .[J].Journal of Natural Gas Chemistry,2012,21:729.
[15]	Ai Sha N L H;Liu J X;Zhao W P;Wang G R Guo H C .[J].J Mol Catal(China),2012,26:257.
[16]	Guisnet M;Gnep N S;Aittaleb D;Doyemet Y J .[J].Applied Catalysis A:General,1992,87:255.
[17]	Guisnet M;Gnep N S .[J].Applied Catalysis A:General,1996,146:33.
[18]	Biscardi J A;Iglesia E .[J].Catalysis Today,1996,31:207.
[19]	Smie(s)ková A;Rojasová E;Hudec P;(S)abo L .[J].Applied Catalysis A:General,2004,268:235.
[20]	Ei-Malki E M;Van Santen R A;Sachtler W M H .[J].Journal of Physical Chemistry B,1999,103:4611.
[21]	Biscardi JA.;Iglesia E.;Meitzner GD. .Structure and density of active Zn species in Zn/H-ZSM5 propane aromatization catalysts[J].Journal of Catalysis,1998(1):192-202.
[22]	Ivanova I I;Kolyagin Y G;Ordomsky V V;Asachenko E V Pasynkova E M Pirogov Y A .[J].Journal of Molecular Catalysis A:Chemical,2009,305:47.
[23]	Kolyagin YG;Ordomsky VV;Khimyak YZ;Rebrov AI;Fajula F;Ivanova II .Initial stages of propane activation over Zn/MFI catalyst studied by in situ NMR and IR spectroscopic techniques[J].Journal of Catalysis,2006(1):122-133.
[24]	Liu J X;Ai Sha N L H;He N;Liu G D Liang C C Zhang X F Guo H C .[J].Journal of Chemical Engineering,2013,218:1.
[25]	Okumura M;Akita T;Haruta M .[J].Catalysis Today,2002,74:265.
[26]	Corma A;Serna P .Chemoselective hydrogenation of nitro compounds with supported gold catalysts[J].Science,2006(5785):332-334.
[27]	Wannakao S;Warakulwit C;Kongpatpanich K;Probst M Limtrakul J .[J].ACS Catal,2012,2:986.
[28]	Sun, C.;Yang, Y.;Du, J.;Qin, F.;Liu, Z.;Shen, W.;Xu, H.;Tang, Y. .Dehydrogenation inhibition on nano-Au/ZSM-5 catalyst: A novel route for anti-coking in methanol to propylene reaction[J].Chemical communications,2012(46):5787-5789.
[29]	Hutchings G J .[J].Catalysis Today,2005,100:55.
[30]	Xin Q;Gao X .[J].Progress in Natural Sciences,1995,5:279.
[31]	Sacaliuc E;Beale A M;Weckhuysen B M;Nijhuis T A .[J].Journal of Catalysis,2007,248:235.
[32]	Lee B;Ma Z;Zhang Z T;Park C Dai S .[J].Microporous and Mesoporous Materials,2009,122:160.
[33]	Wang, L.;Wang, H.;Zhang, W.;Zhang, J.;Lewis, J.P.;Meng, X.;Xiao, F.-S..Aerobic homocoupling of phenylboronic acid on Mg-Al mixed-oxides-supported Au nanoparticles[J].Journal of Catalysis,2013:186-197.

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