Eu~(3+),Tb~(3+)掺杂荧光二氧化硅纳米粒子的合成及其结构、成分和荧光性质的调控
|
摘要
针对目前存在的稀土螯合物掺杂量低、发射吸收波长受到限制等问题,首先用设计好的敏化剂-配体-硅烷偶联剂来螯合稀土离子得到稀土螯合物,然后在反相微乳液中将上述稀土螯合物与正硅酸乙酯(TEOS)共同水解缩聚,合成了稀土掺杂的二氧化硅纳米粒子。通过这种方法,不仅实现了对FSNPs粒径、成分、发射波长的调控,还通过使用不同生色团和稀土离子,获得了对激发波长的调控能力。此外,进一步阐述了稀土掺杂FSNPs中的能量转移过程,提出了一种通过能级调节FSNPs荧光的新方法。
Lanthanides-doped fluorescent silica nanoparticles(FSNPs) were synthesized via a two-step protocol:lanthanide ion was chelated with a conjugation of a chromophore, a ligand and a(3-aminopropyl)triethoxysilane(APTES) molecule. Then the complex was condensed in a water-in-oil microemulsion system together with tetraethyl orthosilicate(TEOS). The existence of coupling silane ensured the bonding in the formation of silica.The influence of water-to-surfactant molar ratio and the amount of prepared conjugation on controlling the particle size and the loading capacity of lanthanides were investigated. Meanwhile, an energy transfer process in lanthanides-doped FSNPs was illustrated by using different chromophores and lanthanides, so that made the excitation wavelength, emission wavelength and fluorescent intensity controllable. Thus, a framework was shaped for the design of silica nanoparticles with diverse fluorescent properties based on engineering the energy levels.In addition, the energy transfer process in rare earth doped FSNPs is further elaborated, and a new method for adjusting the fluorescence of FSNPs by energy level is proposed.
Lanthanides-doped fluorescent silica nanoparticles(FSNPs) were synthesized via a two-step protocol:lanthanide ion was chelated with a conjugation of a chromophore, a ligand and a(3-aminopropyl)triethoxysilane(APTES) molecule. Then the complex was condensed in a water-in-oil microemulsion system together with tetraethyl orthosilicate(TEOS). The existence of coupling silane ensured the bonding in the formation of silica.The influence of water-to-surfactant molar ratio and the amount of prepared conjugation on controlling the particle size and the loading capacity of lanthanides were investigated. Meanwhile, an energy transfer process in lanthanides-doped FSNPs was illustrated by using different chromophores and lanthanides, so that made the excitation wavelength, emission wavelength and fluorescent intensity controllable. Thus, a framework was shaped for the design of silica nanoparticles with diverse fluorescent properties based on engineering the energy levels.In addition, the energy transfer process in rare earth doped FSNPs is further elaborated, and a new method for adjusting the fluorescence of FSNPs by energy level is proposed.
引文
[1] Rosso P, Ye L, Friedrich K, et al. J. Appl. Polym. Sci., 2006,100(3):1849-1855
[2] Slowing I I, Trewyn B G, Giri S, et al. Adv. Funct. Mater.,2007,17(8):1225-1236
[3] Wang L, Zhao W J, Tan W H. Nano Res., 2008,1(2):99-115
[4] Zong C H, Ai K, Zhang G, et al. Anal. Chem., 2011,83(8):3126-3132
[5] Tan H L, Li Q, Ma C J, et al. Biosens. Bioelectron., 2015,63:566-571
[6] Zhang F, Zou M Q, Chen Y, et al. Biosens. Bioelectron.,2014,51:29-35
[7] ZHANG Ze-Fang(张泽芳), YUAN Wei(袁薇), XU Ming(徐明), et al. Chinese J. Inorg. Chem.(无机化学学报), 2018,34(11):1943-1949
[8] Benezra M, Penate-Medina O, Zanzonico P B, et al. J. Clin.Invest., 2011,121(7):2768-2780
[9] Zhao X J, Bagwe R P, Tan W H. Adv. Mater., 2004,16(2):173-176
[10]Diamandis E P, Christopoulos T K. Anal. Chem., 1990,62(22):1149A-1157A
[11]Wu X Y, Liu H J, Liu J Q, et al. Nat. Biotechnol., 2003,21(1):41-46
[12]Medintz I L, Uyeda H T, Goldman E R, et al. Nat. Mater.,2005,4(6):435-446
[13]Michalet X, Pinaud F, Bentolila L, et al. Science, 2005,307(5709):538-544
[14]ZHANG Bing-Bo(张兵波), GONG Xiao-Qun(宫晓群), LIN Ting-Ting(林婷婷), et al. Chem. J. Chinese Universities(高等学校化学学报), 2009,30(2):246-249
[15]Chen Y, Lu Z H. Anal. Chim. Acta, 2007,587(2):180-186
[16]Choi J, Burns A A, Williams R M, et al. J. Biomed. Opt., 2007,12(6):064007
[17]Eliseeva S V, Bünzli J C G. Chem. Soc. Rev., 2010,39(1):189-227
[18]YIN Dong-Guang(尹东光), ZHANG Li(张礼), LIU Bin-Hu(刘斌虎), et al. Chinese J. Inorg. Chem.(无机化学学报),2010,26(3):419-425
[19]Hai X D, Tan M Q, Wang G L, et al. Anal. Sci., 2004,20(2):245-246
[20]Zhang H, Xu Y, Yang W, et al. Chem. Mater., 2007,19(24):5875-5881
[21]Ye Z Q, Tan M Q, Wang G L, et al. J. Mater. Chem., 2004,14(5):851-856
[22]Tan M Q, Wang G L, Hai X D, et al. J. Mater. Chem., 2004,14(19):2896-2901
[23]YIN Dong-Guang(尹东光), ZHANG Li(张礼), LIU Bin-Hu(刘斌虎), et al. Acta Chim. Sinica(化学学报), 2010,68(19):1965-1970
[24]Fedorenko S V, Mustafina A R, Mukhametshina A R, et al.Mater. Sci. Eng. C:Mater. Biol. Appl., 2017,76:551-558
[25]Duarte A P, Mauline L, Gressier M, et al. Langmuir, 2013,29(19):5878-5888
[26]Eliseeva S V, Song B, Vandevyver C D, et al. New J. Chem.,2010,34(12):2915-2921
[27]TAO Dong-Liang(陶栋梁), CUI Yu-Ming(崔玉民), QIAO Rui(乔瑞), et al. Spectroscopy and Spectral Analysis(光谱学与光谱分析), 2011,31(03):723-726
[28]Santra S, Zhang P, Wang K M, et al. Anal. Chem., 2001,73(20):4988-4993
[29]Esquena J, Pons R, Azemar N, et al. Colloids Surf. A, 1997,123:575-586
[30]Yao L, Xu G Y, Dou W L, et al. Colloids Surf. A, 2008,316(1/2/3):8-14
[31]Arriagada F J, Osseo-Asare K. J. Colloid Interface Sci.,1999,211(2):210-220
[32]van Blaaderen A, Vrij A. J. Colloid Interface Sci., 1993,156(1):1-18
[33]Hüsing N, Schubert U, Mezei R, et al. Chem. Mater., 1999,11(2):451-457
[34]Chen S, Hayakawa S, Shirosaki Y, et al. J. Am. Ceram. Soc.,2009,92(9):2074-2082
[35]Chang C L, Fogler H S. Langmuir, 1997,13(13):3295-3307
[36]Ye Z Q, Tan M Q, Wang G L, et al. Anal. Chem., 2004,76(3):513-518
[37]Quici S, Cavazzini M, Marzanni G, et al. Inorg. Chem., 2005,44(3):529-537
[38]Meijer G, de Vries M S, Hunziker H E, et al. J. Chem. Phys.,1990,92(12):7625-7635
[39]S'witlicka-Olszewska A, Klemens T, Nawrot I, et al. J. Lumin.,2016,171:166-175
[40]McCarthy P, Blanchard G. J. Phys. Chem., 1993,97(47):12205-12209
[41]Wu J, Ye Z Q, Wang G L, et al. J. Mater. Chem., 2009,19(9):1258-1264
[42]Shirshahi V, Soltani M. Contrast Media Mol. Imaging, 2015,10(1):1-17
[43]Werts M H, Hofstraat J W, Geurts F A, et al. Chem. Phys.Lett., 1997,276(3/4):196-201
[2] Slowing I I, Trewyn B G, Giri S, et al. Adv. Funct. Mater.,2007,17(8):1225-1236
[3] Wang L, Zhao W J, Tan W H. Nano Res., 2008,1(2):99-115
[4] Zong C H, Ai K, Zhang G, et al. Anal. Chem., 2011,83(8):3126-3132
[5] Tan H L, Li Q, Ma C J, et al. Biosens. Bioelectron., 2015,63:566-571
[6] Zhang F, Zou M Q, Chen Y, et al. Biosens. Bioelectron.,2014,51:29-35
[7] ZHANG Ze-Fang(张泽芳), YUAN Wei(袁薇), XU Ming(徐明), et al. Chinese J. Inorg. Chem.(无机化学学报), 2018,34(11):1943-1949
[8] Benezra M, Penate-Medina O, Zanzonico P B, et al. J. Clin.Invest., 2011,121(7):2768-2780
[9] Zhao X J, Bagwe R P, Tan W H. Adv. Mater., 2004,16(2):173-176
[10]Diamandis E P, Christopoulos T K. Anal. Chem., 1990,62(22):1149A-1157A
[11]Wu X Y, Liu H J, Liu J Q, et al. Nat. Biotechnol., 2003,21(1):41-46
[12]Medintz I L, Uyeda H T, Goldman E R, et al. Nat. Mater.,2005,4(6):435-446
[13]Michalet X, Pinaud F, Bentolila L, et al. Science, 2005,307(5709):538-544
[14]ZHANG Bing-Bo(张兵波), GONG Xiao-Qun(宫晓群), LIN Ting-Ting(林婷婷), et al. Chem. J. Chinese Universities(高等学校化学学报), 2009,30(2):246-249
[15]Chen Y, Lu Z H. Anal. Chim. Acta, 2007,587(2):180-186
[16]Choi J, Burns A A, Williams R M, et al. J. Biomed. Opt., 2007,12(6):064007
[17]Eliseeva S V, Bünzli J C G. Chem. Soc. Rev., 2010,39(1):189-227
[18]YIN Dong-Guang(尹东光), ZHANG Li(张礼), LIU Bin-Hu(刘斌虎), et al. Chinese J. Inorg. Chem.(无机化学学报),2010,26(3):419-425
[19]Hai X D, Tan M Q, Wang G L, et al. Anal. Sci., 2004,20(2):245-246
[20]Zhang H, Xu Y, Yang W, et al. Chem. Mater., 2007,19(24):5875-5881
[21]Ye Z Q, Tan M Q, Wang G L, et al. J. Mater. Chem., 2004,14(5):851-856
[22]Tan M Q, Wang G L, Hai X D, et al. J. Mater. Chem., 2004,14(19):2896-2901
[23]YIN Dong-Guang(尹东光), ZHANG Li(张礼), LIU Bin-Hu(刘斌虎), et al. Acta Chim. Sinica(化学学报), 2010,68(19):1965-1970
[24]Fedorenko S V, Mustafina A R, Mukhametshina A R, et al.Mater. Sci. Eng. C:Mater. Biol. Appl., 2017,76:551-558
[25]Duarte A P, Mauline L, Gressier M, et al. Langmuir, 2013,29(19):5878-5888
[26]Eliseeva S V, Song B, Vandevyver C D, et al. New J. Chem.,2010,34(12):2915-2921
[27]TAO Dong-Liang(陶栋梁), CUI Yu-Ming(崔玉民), QIAO Rui(乔瑞), et al. Spectroscopy and Spectral Analysis(光谱学与光谱分析), 2011,31(03):723-726
[28]Santra S, Zhang P, Wang K M, et al. Anal. Chem., 2001,73(20):4988-4993
[29]Esquena J, Pons R, Azemar N, et al. Colloids Surf. A, 1997,123:575-586
[30]Yao L, Xu G Y, Dou W L, et al. Colloids Surf. A, 2008,316(1/2/3):8-14
[31]Arriagada F J, Osseo-Asare K. J. Colloid Interface Sci.,1999,211(2):210-220
[32]van Blaaderen A, Vrij A. J. Colloid Interface Sci., 1993,156(1):1-18
[33]Hüsing N, Schubert U, Mezei R, et al. Chem. Mater., 1999,11(2):451-457
[34]Chen S, Hayakawa S, Shirosaki Y, et al. J. Am. Ceram. Soc.,2009,92(9):2074-2082
[35]Chang C L, Fogler H S. Langmuir, 1997,13(13):3295-3307
[36]Ye Z Q, Tan M Q, Wang G L, et al. Anal. Chem., 2004,76(3):513-518
[37]Quici S, Cavazzini M, Marzanni G, et al. Inorg. Chem., 2005,44(3):529-537
[38]Meijer G, de Vries M S, Hunziker H E, et al. J. Chem. Phys.,1990,92(12):7625-7635
[39]S'witlicka-Olszewska A, Klemens T, Nawrot I, et al. J. Lumin.,2016,171:166-175
[40]McCarthy P, Blanchard G. J. Phys. Chem., 1993,97(47):12205-12209
[41]Wu J, Ye Z Q, Wang G L, et al. J. Mater. Chem., 2009,19(9):1258-1264
[42]Shirshahi V, Soltani M. Contrast Media Mol. Imaging, 2015,10(1):1-17
[43]Werts M H, Hofstraat J W, Geurts F A, et al. Chem. Phys.Lett., 1997,276(3/4):196-201