Pt supported on Zn modified silicalite-1 zeolite as a catalyst for n-hexane aromatization
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摘要
Platinum(Pt)supported on Zinc(Zn)modified silicalite-1(S-1)zeolite(denoted as Pt-Zn/S-1)was prepared by using a wetness-impregnation method and applied in the n-hexane aromatization reaction for the first time.Both Lewis and Br?nsted acid sites were detected in Pt-Zn/S-1 catalyst by means of FT-IR adsorption of NH_3 experiment,which were identified as mostly weak and medium ones.Besides,Pt and Zn species showed strong interaction,as revealed by the TPR(Temperature-programmed reduction)and XPS(X-ray photoelectron spectroscopy)experiments.Pt-Zn/S-1 catalyst exhibited excellent aromatization function rather than isomerization and cracking side reactions in the conversion of n-hexane.Pulse experimental study showed that 75.6% of n-hexane conversion and 76.8% of benzene selectivity were obtained over Pt_(0.1)-Zn_(6.0)/S-1 catalyst at 550℃ and under atmospheric pressure.By spectroscopy tests and pulse experimental results,it was concluded that the n-hexane aromatization over Pt-Zn/S-1 catalyst follows a metal-acid bifunctional mechanism.Furthermore,with the assistance of Zn,the electron-deficient Pt species in Pt-Zn/S-1 showed good sulfur tolerance performance.
Platinum(Pt)supported on Zinc(Zn)modified silicalite-1(S-1)zeolite(denoted as Pt-Zn/S-1)was prepared by using a wetness-impregnation method and applied in the n-hexane aromatization reaction for the first time.Both Lewis and Br?nsted acid sites were detected in Pt-Zn/S-1 catalyst by means of FT-IR adsorption of NH_3 experiment,which were identified as mostly weak and medium ones.Besides,Pt and Zn species showed strong interaction,as revealed by the TPR(Temperature-programmed reduction)and XPS(X-ray photoelectron spectroscopy)experiments.Pt-Zn/S-1 catalyst exhibited excellent aromatization function rather than isomerization and cracking side reactions in the conversion of n-hexane.Pulse experimental study showed that 75.6% of n-hexane conversion and 76.8% of benzene selectivity were obtained over Pt_(0.1)-Zn_(6.0)/S-1 catalyst at 550℃ and under atmospheric pressure.By spectroscopy tests and pulse experimental results,it was concluded that the n-hexane aromatization over Pt-Zn/S-1 catalyst follows a metal-acid bifunctional mechanism.Furthermore,with the assistance of Zn,the electron-deficient Pt species in Pt-Zn/S-1 showed good sulfur tolerance performance.
Platinum(Pt)supported on Zinc(Zn)modified silicalite-1(S-1)zeolite(denoted as Pt-Zn/S-1)was prepared by using a wetness-impregnation method and applied in the n-hexane aromatization reaction for the first time.Both Lewis and Br?nsted acid sites were detected in Pt-Zn/S-1 catalyst by means of FT-IR adsorption of NH_3 experiment,which were identified as mostly weak and medium ones.Besides,Pt and Zn species showed strong interaction,as revealed by the TPR(Temperature-programmed reduction)and XPS(X-ray photoelectron spectroscopy)experiments.Pt-Zn/S-1 catalyst exhibited excellent aromatization function rather than isomerization and cracking side reactions in the conversion of n-hexane.Pulse experimental study showed that 75.6% of n-hexane conversion and 76.8% of benzene selectivity were obtained over Pt_(0.1)-Zn_(6.0)/S-1 catalyst at 550℃ and under atmospheric pressure.By spectroscopy tests and pulse experimental results,it was concluded that the n-hexane aromatization over Pt-Zn/S-1 catalyst follows a metal-acid bifunctional mechanism.Furthermore,with the assistance of Zn,the electron-deficient Pt species in Pt-Zn/S-1 showed good sulfur tolerance performance.
引文
[1]G.Q.Zhang,X.Zhang,T.Bai,T.F.Chen,W.T Fan,J.Energy Chem.24(2015)108-118.
[2]N.K.Mal,M.Sasidharan,M.Matsukata,S.Sivasanker,A.V.Ramasawamy,Stud.Surf.Sci.Catal.154(2004)2403-2410.
[3]P.Meriaudeau,C.Naccache,Catal.Rev.Sci.Eng.39(1 and 2)(1997)5-48.
[4]K.Lee,M.Choi,J.Catal.340(2016)66-75.
[5]M.Kumar,A.K.Saxena,B.S.Negi,N.Viswanadham,Catal.Today.130(2008)501-508.
[6]G.Jacobs,W.E.Alvarez,D.E.Resasco,Appl.Catal.A 206(2001)267-282.
[7]S.J.Tauster,J.J.Steger,J.Catal.125(1990)387-389.
[8]K.G.Azzam,G.Jacobs,W.D.Shafer,B.H.Davis,J.Catal 270(2010)242-248.
[9]G.Jacobs,C.L.Padro,D.E.Resasco,J.Catal.179(1998)43-55.
[10]G.Jacobs,F.Ghadiali,A.Pisanu,C.L.Padro,A.Borgna,W.E.Alvarez,D.E.Resasco,J.Catal.191(2000)116-127.
[11]V.Bolis,C.Busco,S.Bordiga,P.Ugliengo,C.Lamberti,A.Zecchina,Appl.Surf.Sci.196(2002)56-70.
[12]G.P.Heitmann,G.Dahlhoff,W.F.H?lderich,J.Catal.186(1999)12-19.
[13]H.Ichihashi,H.Sato,Appl.Catal A:Gen.221(2001)359-366.
[14]H.Ichihashi,M.Ishida,A.Shiga,M.Kitamura,T.Suzuki,K.Suenobu,K.Sugita,Catal.Surv.Asia.7(2003)261-270.
[15]G.D.Liu,J.X.Liu,N.He,C.L.Miao,J.L.Wang,Q.Xin,H.C.Guo,RSC Adv.8(2018)18663-18671.
[16]W.F.Elseviers,H.Verelst,Fuel.78(1999)601-612.
[17]L.Li,D.L.King,Catal.Today.116(2006)537-541.
[18]J.A.Fouts,B.Fowler,P.J.Shiller,G.L.Doll,Surf.Coat.Tech.314(2017)55-66.
[19]J.Silvestre-Albero,J.C.Serrano-Ruiz,A.Sepu′lveda-Escribano,F.Rodr?′guez-Reinoso,Appl.Catal.A General 292(2005)244-251.
[20]M.Consonni,D.Jokic,D.Y.Murzin,R.Touroude,J.Catal.188(1999)165-175.
[21]L.Q.Wang,X.S.Wang,X.W.Guo,Chin.J.Catal.22(2001)513-514.
[22]Y.M.Ni,W.Y.Peng,M.Sun A,W.L.Mo,J.L.Hu,T.Li,G.X.Li,J.Ind.Eng.Chem.16(2010)503-505.
[23]H.A.Zaidi,K.K.Pant,Catal.Today.96(2004)155-160.
[24]Y.G.Kolyagin,V.V.Ordomsky,Y.Z.Khimyak,A.I.Rebrovc,F.Fajulad,I.I.Ivanova,J.Catal.238(2006)122-133.
[25]J Chen,Z Feng,P Ying,C Li,J.Phys.Chem.B.108(2004)12669-12676.
[26]L.W.Ho,C.P.Hwang,J.F.Lee,I.Wang,C.T.Yeh,J.Mol.Catal.A-Chem.136(1998)293-299.
[27]C.P.Hwang,C.T.Yeh,J.Mol.Catal.A-Chem.112(1996)295-302.
[28]Y.D.Wang,Z.C.Tao,B.S.Wu,J.Xu,C.F.Huo,K.Li,H.M.Chen,Y.Yang,Y.W.Li,J.Catal.322(2015)1-13.
[29]M.Consonni,D.Jokic,D.Yu Murzin,R.Touroude,J.Catal.188(1999)165-175.
[30]J.A.Biscardi,G.D.Meitzner,E.Iglesia,J.Catal.179(1998)192-202.
[31]C.D.Wagner,W.M.Riggs,L.E.Davos,J.F.Moulder,G.E.Murlenberg,Handbook of X-ray Photoelectron Spectroscopy,Perkin-Elmer Corp.,Minnesota,1979.
[32]B.Peplinski,W.Unger,I.Grohmann,Appl.Surf.Sci.62(1992)115-129.
[33]T.Kosec,I.Milosev,B.Pihlar,Appl.Surf.Sci.253(2007)8863-8873.
[34]I.Milosev,H.H.Strehblow,J.Electrochem.Soc.150(2003)B517-B524.
[35]F.Yin,A.L.Blumenfeld,V.Gruver,J.J.Fripiat,J.Phys.Chem.B.101(1997)1824-1830.
[36]W.Zhang,P.G.Smirniotis,M.Gangoda,R.N.Bose,J.Phys.Chem.B.104(2000)4122-4129.
[37]V.S.Escribanoa,T.Montanarib,G.Busca,Appl.Catal.B:Environmental.58(2005)19-23.
[38]G.V.A.Martins,G.Berlie,C.Bisio,S.Coluccia,H.O.Pastore,L.Marchese,J.Phys.Chem.C.112(2008)7193-7200.
[39]S.Sivasanker,S.R.Padalkar,Appl.Catal.39(1988)123-126.
[40]P.G.Smirniotis,E.Ruckenstein,Appl.Catal.123(1995)59-88.
[41]B.H.Davis,P.B.Venuto,J.Catal.15(1969)363-372.
[42]S.J.Tauster,J.J.Steger,J.Catal.125(1990)387-389.
[43]F.J.Maldonado-Hódar,Appl.Catal.A Gen.408(2011)156-162.
[44]A.Trunschke,D.L.Hoang,J.Radnik,K.W.Brzezinka,A.Brückner,H.Lieske,Appl.Catal.A.208(2001)381-392.
[45]P.G.Smirniotis,E.Ruckenstein,J.Catal.140(1993)526-542.
[46]Z.Paal,Z.Q.Zhan,I.Manninger,W.M.H Sachtler,J.Catal.155(1995)43-51.
[47]J.Zheng,J.L.Dong,Q.H.Xu,Y.Liu,A.Z.Yan,Appl.Catal.A Gen.126(1995)141-152.
[48]J.Zheng,T.Schmauk,E.Roduner,J.L.Dong,Q.H.Xu,J.Mol.Catal.A Chem.171(2001)181-190.
[2]N.K.Mal,M.Sasidharan,M.Matsukata,S.Sivasanker,A.V.Ramasawamy,Stud.Surf.Sci.Catal.154(2004)2403-2410.
[3]P.Meriaudeau,C.Naccache,Catal.Rev.Sci.Eng.39(1 and 2)(1997)5-48.
[4]K.Lee,M.Choi,J.Catal.340(2016)66-75.
[5]M.Kumar,A.K.Saxena,B.S.Negi,N.Viswanadham,Catal.Today.130(2008)501-508.
[6]G.Jacobs,W.E.Alvarez,D.E.Resasco,Appl.Catal.A 206(2001)267-282.
[7]S.J.Tauster,J.J.Steger,J.Catal.125(1990)387-389.
[8]K.G.Azzam,G.Jacobs,W.D.Shafer,B.H.Davis,J.Catal 270(2010)242-248.
[9]G.Jacobs,C.L.Padro,D.E.Resasco,J.Catal.179(1998)43-55.
[10]G.Jacobs,F.Ghadiali,A.Pisanu,C.L.Padro,A.Borgna,W.E.Alvarez,D.E.Resasco,J.Catal.191(2000)116-127.
[11]V.Bolis,C.Busco,S.Bordiga,P.Ugliengo,C.Lamberti,A.Zecchina,Appl.Surf.Sci.196(2002)56-70.
[12]G.P.Heitmann,G.Dahlhoff,W.F.H?lderich,J.Catal.186(1999)12-19.
[13]H.Ichihashi,H.Sato,Appl.Catal A:Gen.221(2001)359-366.
[14]H.Ichihashi,M.Ishida,A.Shiga,M.Kitamura,T.Suzuki,K.Suenobu,K.Sugita,Catal.Surv.Asia.7(2003)261-270.
[15]G.D.Liu,J.X.Liu,N.He,C.L.Miao,J.L.Wang,Q.Xin,H.C.Guo,RSC Adv.8(2018)18663-18671.
[16]W.F.Elseviers,H.Verelst,Fuel.78(1999)601-612.
[17]L.Li,D.L.King,Catal.Today.116(2006)537-541.
[18]J.A.Fouts,B.Fowler,P.J.Shiller,G.L.Doll,Surf.Coat.Tech.314(2017)55-66.
[19]J.Silvestre-Albero,J.C.Serrano-Ruiz,A.Sepu′lveda-Escribano,F.Rodr?′guez-Reinoso,Appl.Catal.A General 292(2005)244-251.
[20]M.Consonni,D.Jokic,D.Y.Murzin,R.Touroude,J.Catal.188(1999)165-175.
[21]L.Q.Wang,X.S.Wang,X.W.Guo,Chin.J.Catal.22(2001)513-514.
[22]Y.M.Ni,W.Y.Peng,M.Sun A,W.L.Mo,J.L.Hu,T.Li,G.X.Li,J.Ind.Eng.Chem.16(2010)503-505.
[23]H.A.Zaidi,K.K.Pant,Catal.Today.96(2004)155-160.
[24]Y.G.Kolyagin,V.V.Ordomsky,Y.Z.Khimyak,A.I.Rebrovc,F.Fajulad,I.I.Ivanova,J.Catal.238(2006)122-133.
[25]J Chen,Z Feng,P Ying,C Li,J.Phys.Chem.B.108(2004)12669-12676.
[26]L.W.Ho,C.P.Hwang,J.F.Lee,I.Wang,C.T.Yeh,J.Mol.Catal.A-Chem.136(1998)293-299.
[27]C.P.Hwang,C.T.Yeh,J.Mol.Catal.A-Chem.112(1996)295-302.
[28]Y.D.Wang,Z.C.Tao,B.S.Wu,J.Xu,C.F.Huo,K.Li,H.M.Chen,Y.Yang,Y.W.Li,J.Catal.322(2015)1-13.
[29]M.Consonni,D.Jokic,D.Yu Murzin,R.Touroude,J.Catal.188(1999)165-175.
[30]J.A.Biscardi,G.D.Meitzner,E.Iglesia,J.Catal.179(1998)192-202.
[31]C.D.Wagner,W.M.Riggs,L.E.Davos,J.F.Moulder,G.E.Murlenberg,Handbook of X-ray Photoelectron Spectroscopy,Perkin-Elmer Corp.,Minnesota,1979.
[32]B.Peplinski,W.Unger,I.Grohmann,Appl.Surf.Sci.62(1992)115-129.
[33]T.Kosec,I.Milosev,B.Pihlar,Appl.Surf.Sci.253(2007)8863-8873.
[34]I.Milosev,H.H.Strehblow,J.Electrochem.Soc.150(2003)B517-B524.
[35]F.Yin,A.L.Blumenfeld,V.Gruver,J.J.Fripiat,J.Phys.Chem.B.101(1997)1824-1830.
[36]W.Zhang,P.G.Smirniotis,M.Gangoda,R.N.Bose,J.Phys.Chem.B.104(2000)4122-4129.
[37]V.S.Escribanoa,T.Montanarib,G.Busca,Appl.Catal.B:Environmental.58(2005)19-23.
[38]G.V.A.Martins,G.Berlie,C.Bisio,S.Coluccia,H.O.Pastore,L.Marchese,J.Phys.Chem.C.112(2008)7193-7200.
[39]S.Sivasanker,S.R.Padalkar,Appl.Catal.39(1988)123-126.
[40]P.G.Smirniotis,E.Ruckenstein,Appl.Catal.123(1995)59-88.
[41]B.H.Davis,P.B.Venuto,J.Catal.15(1969)363-372.
[42]S.J.Tauster,J.J.Steger,J.Catal.125(1990)387-389.
[43]F.J.Maldonado-Hódar,Appl.Catal.A Gen.408(2011)156-162.
[44]A.Trunschke,D.L.Hoang,J.Radnik,K.W.Brzezinka,A.Brückner,H.Lieske,Appl.Catal.A.208(2001)381-392.
[45]P.G.Smirniotis,E.Ruckenstein,J.Catal.140(1993)526-542.
[46]Z.Paal,Z.Q.Zhan,I.Manninger,W.M.H Sachtler,J.Catal.155(1995)43-51.
[47]J.Zheng,J.L.Dong,Q.H.Xu,Y.Liu,A.Z.Yan,Appl.Catal.A Gen.126(1995)141-152.
[48]J.Zheng,T.Schmauk,E.Roduner,J.L.Dong,Q.H.Xu,J.Mol.Catal.A Chem.171(2001)181-190.