微通道连续合成UiO-66系列改性MOF材料
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摘要
采用内交叉指型微反应器连续合成Ui O-66材料.连续微通道法强化了物料之间的混合,极大提高了生产效率,晶体产物呈六面体形,粒径在100 nm以下.考察了温度、总进料流量和停留时间等条件对合成过程及产物的影响.结果表明,升高温度有助于晶粒的生长;随着总进料流量增大,晶体粒径减小;晶体的形成需要一定的停留时间,超过该停留时间,晶体粒径不再增大.通过优化实验条件,可以实现系列纳米级Ui O-66-X材料(X=NH_2,NO_2,Br)的连续合成.
Zirconium based metal-organic framework UiO-66 was synthesized continuously by microfluidic method. Compared with the traditional solvothermal synthesis in batch reactors,microfluidic synthesis is more efficient. It has the advantages in highly efficient mixing and heat transfer,thus lead to enhanced reaction rates. Microfluidic synthesis can obtain uniform hexahedral crystalline products in nanometer range( less than100 nm). The influences of temperature,total flowrate and residence time on the obtained products were investigated. Higher temperature benefited the growth of crystal. When flowrate increased,crystal sizes of UiO-66 synthesized by microfluidic method decreased. Crystal growth required sufficient residence time( 20 min),but if the residence time was prolonged further,the crystal particle size would not change any more. By optimizing the synthetic parameters,UiO-66 modified with different functional groups,UiO-66-X( X =NH_2,NO_2,Br),could be synthesized continuously by microfluidic synthesis.
Zirconium based metal-organic framework UiO-66 was synthesized continuously by microfluidic method. Compared with the traditional solvothermal synthesis in batch reactors,microfluidic synthesis is more efficient. It has the advantages in highly efficient mixing and heat transfer,thus lead to enhanced reaction rates. Microfluidic synthesis can obtain uniform hexahedral crystalline products in nanometer range( less than100 nm). The influences of temperature,total flowrate and residence time on the obtained products were investigated. Higher temperature benefited the growth of crystal. When flowrate increased,crystal sizes of UiO-66 synthesized by microfluidic method decreased. Crystal growth required sufficient residence time( 20 min),but if the residence time was prolonged further,the crystal particle size would not change any more. By optimizing the synthetic parameters,UiO-66 modified with different functional groups,UiO-66-X( X =NH_2,NO_2,Br),could be synthesized continuously by microfluidic synthesis.
引文
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[30]Vanlenzano L.,Civalleri B.,Chavan S.,Bodiga S.,Nilsen M.H.,Jakobsen S.,Lillerud K.P.,Lamberti C.,Chem.Mater.,2011,23(7),1700-1718
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[34]Kim M.B.,Kim K.M.,Kim T.H.,Yoon T.U.,Kim E.J.,Kim J.H.,Bae Y.S.,Chem.Eng.J.,2018,339,223-229
[2]Cavka J.H.,Jakobsen S.,Olsbye U.,Guillou N.,Lamberti C.,Bordiga S.,Lillerud K.P.,J.Am.Chem.Soc.,2008,130(42),13850-13851
[3]Wang L.P.,Wang G.Y.,J.Mol.Catal.(China),2015,29(3),275-288(王丽苹,王公应.分子催化,2015,29(3),275-288)
[4]Luan Y.,Qi Y.,Jin Z.K.,Peng X.,Gao H.Y.,Wang G.,RSC Adv.,2015,5(25),19273-19278
[5]Eddaoudi M.,Kim J.,Rosi N.,Vodak D.,Wachter J.,O’Keeffe M.,Yaghi O.M.,Science,2002,295(5554),469-472
[6]Kitagawa S.,Kitaura R.,Noro S.,Angew.Chem.Int.Ed.,2004,43(18),2334-2375
[7]Konstas K.,Taylor J.W.,Thronton A.W.,Doherty C.M.,Lim W.X.,Bastow T.J.,Kennedy D.F.,Wood C.D.,Cox B.J.,Hill J.M.,Hill A.J.,Hill M.R.,Angew.Chem.Int.Ed.,2012,51(27),6639-6642
[8]Sumida K.,Rogow D.L.,Mason J.A.,Mc Donald T.M.,Bloch E.D.,Herm Z.R.,Bae T.H.,Long J.R.,Chem.Rev.,2012,112(2),724-781
[9]Horcajada P.,Chalati T.,Serre C.,Gillet B.,Sebrie C.,Baati T.,Eubank J.F.,Heurtaux D.,Clayette P.,Kreuz C.,Chang J.S.,Hwang Y.K.,Marsaud V.,Bories P.N.,Cynober L.,Gil S.,Ferey G.,Couvreur P.,Gref R.,Nat.Mater.,2010,9(2),172-178
[10]Liu D.M.,Lu K.D.,Poon C.,Lin W.B.,Inorg.Chem.,2014,53(4),1916-1924
[11]Wang F.X.,Wang C.C.,Wang P.,Xing B.Z.,Chin.J.Inorg.Chem.,2017,33(5),713-737(王茀学,王崇臣,王鹏,邢碧枞.无机化学学报,2017,33(5),713-737)
[12]Bai Y.,Dou Y.B.,Xie L.H.,Rutledge W.,Li J.R.,Zhou H.C.,Chem.Soc.Rev.,2016,45,2327-2367
[13]Yan X.D.,Wang K.,Xu X.C.,Wang S.H.,Ning Q.,Xiao W.M.,Zhang N.,Chen Z.J.,Chen C.,Inorg.Chem.,2018,57,8033-8036
[14]Zhang M.W.,Chen Y.P.,Bosch M.,Gentle T.,Wang K.C.,Feng D.W.,Wang Z.Y.U.,Zhou H.C.,Angew.Chem.Int.Ed.,2014,53,815-818
[15]Kandiah M.,Nilsen M.H.,Usseglio S.,Jakobsen S.,Olsbye U.,Tilset M.,Larabi C.,Quadrelli E.A.,Bonino F.,Lillerud K.P.,Chem.Mater.,2010,22(24),6632-6640
[16]Ferey G.,Chem.Soc.Rev.,2008,37,191-214
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[19]MAE K.,Chem.Eng.Sci.,2007,62(18-20),4842-4851
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[21]Luo G.S.,Wang K.,Wang P.J.,CIESC J.,2014,65(7),2563-2573(骆广生,王凯,王佩坚.化工学报,2014,65(7),2563-2573)
[22]Cao Y.,Yang H.,Inorg.Chem.Ind.,2011,43(5),7-10(曹寅,杨晖.无机盐工业,2011,43(5),7-10)
[23]Jovanovic J.,Rebrov E.V.,Nuhuis T.A.,Kreutzer M.T.,Hessel V.,Schouten J.C.,Ind.Eng.Chem.Res.,2011,51(2),1015-1026
[24]He W.,Fang Z.,Chen K.T.,Wang Z.D.,Guo K.,Chin.J.Appl.Chem.,2013,30(12),1375-1385(何伟,方正,陈克涛,万志东,郭凯.应用化学,2013,30(12),1375-1385)
[25]Rubio-Martinez M.,Batten M.P.,Polyzos A.Carey K.,Mardel J.I.,Lim K.S.,Hill M.R.,Sci.Rep.,2014,4,5443
[26]Wang Y.,Li L.J.,Dai P.C.,Yan L.T.,Cao L.,Gu X.,Zhao X.B.,J.Mater.Chem.A,2017,5(42),22372-22379
[27]Liu H.F.,Wang F.C.,Wu T.,Gong X.,Yu Z.H.,J.East China university Sci.Technol.,1999,3,227-232(刘海峰,王辅臣,吴韬,龚欣,于遵宏.华东理工大学学报,1999,3,227-232)
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[29]Han Y.T.,Liu M.,Li K.Y.,Zuo Y.,Xu S.T.,Zhang G.L.,Song C.S.,Zhang Z.C.,Guo X.W.,Cryst.Eng.Comm.,2015,17(33),6434-6440
[30]Vanlenzano L.,Civalleri B.,Chavan S.,Bodiga S.,Nilsen M.H.,Jakobsen S.,Lillerud K.P.,Lamberti C.,Chem.Mater.,2011,23(7),1700-1718
[31]Brar T.,France P.,Smirniotis P.G.,Ind.Eng.Chem.Res.,2001,40,1133-1139
[32]Ju J.X.,Zeng C.F.,Zhang L.X.,Xu N.P.,Chem.Eng.J.,2006,116,115-121
[33]Ren Z.L.,Lu C.Y.,Wang A.J.,Wang Y.,CIESC J.,2017,68(6),2611-2617(任郑玲,卢晨阳,王安杰,王瑶.化工学报,2017,68(6),2611-2617)
[34]Kim M.B.,Kim K.M.,Kim T.H.,Yoon T.U.,Kim E.J.,Kim J.H.,Bae Y.S.,Chem.Eng.J.,2018,339,223-229