Synthesis of Fe_3O_4@SiO_2-Au/Cu magnetic nanoparticles and its efficient catalytic performance for the Ullmann coupling reaction of bromamine acid
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摘要
Novel magnetic core/shell bimetallic Au/Cu nanoparticles(Fe_3O_4@SiO_2-Au/Cu NPs) were prepared using SiO_2-coated iron oxide(Fe_3O_4@SiO_2) as a supported material. The magnetic Fe_3O_4 colloidal nanocrystal clusters(CNCs) as nano-core were modified with a silica coating for improvement stability and superficial area of the Au-Cu particles. The morphological structure and chemical composition of the Fe_3O_4@SiO_2-Au/Cu NPs were characterized with high-resolution transmission electron microscopy(HRTEM), energy-dispersive X-ray(EDX) and X-ray photoelectron spectroscopy(XPS) analyses. The Au and Cu NPs were deposited on the SiO_2 surface in a highly dense and well dispersed manner with an average size of approximately 5 nm. The Fe_3O_4@SiO_2-Au/Cu NPs as magnetic nano-catalysts were applied to the Ullmann coupling reaction of bromamine acid to synthesize 4,40-diamino-1,10-dianthraquinonyl-3,30-disulfonic acid(DAS). The prepared Fe_3O_4@SiO_2-Au/Cu NPs exhibited efficient catalytic activity with higher conversion and selectivity. A bromamine acid conversion of 97.35% and selectivity for DAS of 88.67% were obtained in aqueous medium. The magnetic nano-catalysts can be readily separated from the reaction system and reused. This new nano-catalytic reaction represents a useful and attractive cleaner production system. The new catalyst system has important and potential applications in dye and pigment industry.
Novel magnetic core/shell bimetallic Au/Cu nanoparticles(Fe_3O_4@SiO_2-Au/Cu NPs) were prepared using SiO_2-coated iron oxide(Fe_3O_4@SiO_2) as a supported material. The magnetic Fe_3O_4 colloidal nanocrystal clusters(CNCs) as nano-core were modified with a silica coating for improvement stability and superficial area of the Au-Cu particles. The morphological structure and chemical composition of the Fe_3O_4@SiO_2-Au/Cu NPs were characterized with high-resolution transmission electron microscopy(HRTEM), energy-dispersive X-ray(EDX) and X-ray photoelectron spectroscopy(XPS) analyses. The Au and Cu NPs were deposited on the SiO_2 surface in a highly dense and well dispersed manner with an average size of approximately 5 nm. The Fe_3O_4@SiO_2-Au/Cu NPs as magnetic nano-catalysts were applied to the Ullmann coupling reaction of bromamine acid to synthesize 4,40-diamino-1,10-dianthraquinonyl-3,30-disulfonic acid(DAS). The prepared Fe_3O_4@SiO_2-Au/Cu NPs exhibited efficient catalytic activity with higher conversion and selectivity. A bromamine acid conversion of 97.35% and selectivity for DAS of 88.67% were obtained in aqueous medium. The magnetic nano-catalysts can be readily separated from the reaction system and reused. This new nano-catalytic reaction represents a useful and attractive cleaner production system. The new catalyst system has important and potential applications in dye and pigment industry.
Novel magnetic core/shell bimetallic Au/Cu nanoparticles(Fe_3O_4@SiO_2-Au/Cu NPs) were prepared using SiO_2-coated iron oxide(Fe_3O_4@SiO_2) as a supported material. The magnetic Fe_3O_4 colloidal nanocrystal clusters(CNCs) as nano-core were modified with a silica coating for improvement stability and superficial area of the Au-Cu particles. The morphological structure and chemical composition of the Fe_3O_4@SiO_2-Au/Cu NPs were characterized with high-resolution transmission electron microscopy(HRTEM), energy-dispersive X-ray(EDX) and X-ray photoelectron spectroscopy(XPS) analyses. The Au and Cu NPs were deposited on the SiO_2 surface in a highly dense and well dispersed manner with an average size of approximately 5 nm. The Fe_3O_4@SiO_2-Au/Cu NPs as magnetic nano-catalysts were applied to the Ullmann coupling reaction of bromamine acid to synthesize 4,40-diamino-1,10-dianthraquinonyl-3,30-disulfonic acid(DAS). The prepared Fe_3O_4@SiO_2-Au/Cu NPs exhibited efficient catalytic activity with higher conversion and selectivity. A bromamine acid conversion of 97.35% and selectivity for DAS of 88.67% were obtained in aqueous medium. The magnetic nano-catalysts can be readily separated from the reaction system and reused. This new nano-catalytic reaction represents a useful and attractive cleaner production system. The new catalyst system has important and potential applications in dye and pigment industry.
引文
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[2]M.Banach,J.Pulit-Prociak,J.Clean.Prod.141(2017)1030-1039.
[3]K.Tian,W.J.Liu,S.Zhang,H.Jiang,Green Chem.18(2016)5643-5650.
[4]T.Mitsudome,K.Miyagawa,Z.Maeno,et al.,Angew.Chem.Int.Ed.129(2017)9509-9513.
[5]A.Lehoux,L.Ramos,P.Beaunier,et al.,Adv.Funct.Mater.22(2012)4900-4908.
[6]X.Liu,A.Wang,L.Li,et al.,J.Catal.278(2011)288-296.
[7]X.M.Fu,Z.J.Liu,S.X.Cai,et al.,Chin.Chem.Lett.27(2016)920-926.
[8]S.Bhattacharjee,C.S.Tan,J.Clean.Prod.156(2017)203-213.
[9]X.Weng,M.Guo,F.Luo,Z.Chen,J.Chem.Eng.308(2017)904-911.
[10]M.Comotti,W.C.Li,B.Spliethoff,F.Schiith,J.Am.Chem.Soc.128(2006)917-924.
[11]T.Tabakova,L.Ilieva,P.Petrova,et al.,Chem.Eng.J.260(2015)133-141.
[12]F.Benaskar,N.Patil,V.Engels,et al.,Chem.Eng.J.207(2012)426-439.
[13]V.Engels,F.Benaskar,N.Patil,et al.,Org.Process Res.Dev.14(2010)644-649.
[14]K.J.Shi,X.Zhang,C.H.Shu,et al.,Chem.Commun.52(2016)8726-8729.
[15]T.C.Ou,F.W.Chang,L.S.Roselin,J.Mol,Catal.A:Chem.293(2008)8-16.
[16]X.M.Liao,V.Pitchon,P.H.Cuong,W.Chu,V.Caps,Chin.Chem.Lett.28(2017)293-296.
[17]M.Y.Liu,W.Zhou,T.Wang,et al.,Chem.Commun.53(2016)4694-4697.
[18]S.Hu,Y.Guan,Y.Wang,H.Han,Appl.Energ.88(2011)2685-2690.
[19]J.Y.Zhang,X.Huang,Q.Y.Shen,J.Y.Wang,G.H.Song,Chin.Chem.Lett 29(2018)197-200.
[20]A.C.Alba-Rubio,J.Santamaria-Gonzalez,J.M.Merida-Robles,et al.,Catal.Today 149(2010)281-287.
[21]Z.Abbasi,S.Rezayati,M.Bagheri,R.Hajinasiri,Chin.Chem.Lett.28(2017)75-82.
[22]L.L.Kong,L.Y.Fan,Chin.Chem.Lett.27(2016)827-831.
[23]F.Karci,N.Sener,M.Yamac,I.Sener,A.Demircali,Dyes Pigments 80(2009)47-52.
[24]M.M.M.Raposo,M.C.R.Castro,M.Belsley,A.M.C.Fonseca,Dyes Pigments 91(2011)454-465.
[25]A.Asghar,A.A.A.Raman,W.M.A.W.Daud,J.Clean.Prod.87(2015)826-838.
[26]C.W.Qian,W.L.Lv,Q.S.Zong,M.Y.Wang,D.Fang,Chin.Chem.Lett.25(2014)337-340.
[27]F.Benaskar,V.Engels,N.G.Patil,et al.,Ind.Eng.Chem.Res.52(2013)18206-18214.
[28]R.N.Dhital,C.Kamonsatikul,E.Somsook,et al.,J.Am.Chem.Soc.134(2012)20250-20253.
[29]A.Kamal,V.Srinivasulu,B.Seshadri,et al.,Green Chem.14(2012)2513-2522.