Pd(Ⅱ)-Directed Layer-by-layer Assembly of Multiporphyrin Arrays on Silica Nanoparticle Surfaces for Photocurrent Generation and Photochromism of Viologens†

doi:10.7503/cjcu20160840

Abstract

Abstract:

Pyridyl-functionalized silica nanoparticles(nanoSiO₂BPy) were prepared, on the surfaces of which the Pd(Ⅱ)-directed multiporphyrin arrays were constructed by using the layer-by-layer(LBL) technique with zinc tetrapyridylporphyrin(ZnTPyP) as multi-dentate linkers to produce the nanoSiO₂BPy@(Pd/ZnTPyP)_n hybrid material. Thermogravimetric analysis revealed a mass loss of approximately 17% of the total mass that was attributed to the decomposition of organic species in the nanoSiO₂BPy@(Pd/ZnTPyP)₃ hybrid. For the ZnTPyP in the hybrids, the Soret absorption band appeared at about 426 nm, the fluorescent emission bands appeared at about 605 and 655 nm, and the emission lifetime was approximately 1.78 ns. All these data were much similar to those of ZnTPyP in the dilute DMSO solutions, suggesting that the porphyrin-porphyrin interactions were weak and no porphyrin aggregates formed in the hybrid. The silica nanoparticle sizes slightly increased from 10—16 nm to 15—20 nm, which was attributed to the fact that the multiporphyrin arrays were immobilized on the particle surfaces. Cyclic voltammograms of the hybrid in the casting films revealed two couples of redox peaks in the potential range of -0.6—-2.4 V(vs. Ag/AgCl), corresponding to the electron transfer processes of porphyrin oxidation. Finally, the indium tin oxide electrodes covered with the nanoSiO₂BPy@(Pd/ZnTPyP)₃ hybrid were used as the photosensitizers for the light-induced current generation and photochromism of ethyl viologens.

Key words: Multiporphyrin array, Hybrid material, Layer-by-layer assembly, Photocurrent, Photochromism

CLC Number:

O647

TrendMD:

HE Wenli, CHEN Meng, QIAN Dongjin. Pd(Ⅱ)-Directed Layer-by-layer Assembly of Multiporphyrin Arrays on Silica Nanoparticle Surfaces for Photocurrent Generation and Photochromism of Viologens^†[J]. Chem. J. Chinese Universities, 2017, 38(9): 1654.

Figures/Tables 10

Fig.1 Surface modification of nanoSiO2 particles and Pd(Ⅱ)-directed self-assembly of nanoSiO2BPy@(Pd/ZnTPyP)n hybrid material

Fig.2 FTIR spectra of nanoSiO2BenCl(a), nanoSiO2BPy(b) and nanoSiO2BPy@(Pd/ZnTPyP)3(c) hybrid materials

Fig.3 Thermogravimetric curves of nanoSiO2BenCl(a), nanoSiO2BPy(b) and nanoSiO2BPy@(Pd/ZnTPyP)3(c) in air

Fig.4 Absorption spectra of ZnTPyP(a) and nanoSiO2BPy@(Pd/ZnTPyP)3 hybrid(b) in DMSO

Fig.5 High-resolution XPS spectra of the nano-SiO2BPy@(Pd/ZnTPyP)3 hybrid

Fig.6 FETEM images of nanoSiO2BenCl(A) and nanoSiO2BPy@(Pd/ZnTPyP)3(B) hybrid Insets: high resolution FETEM images.

Fig.7 Fluorescent emission spectra(A) and time-resolved emission decay(B) of ZnTPyP(a) and nanoSiO2BPy@(Pd/ZnTPyP)3 hybrid(b) in DMSO

Fig.8 Cyclic voltammograms of the glass carbon electrodes covered with ZnTPyP(a) and nanoSiO2BPy@(Pd/ZnTPyP)3(b) casting films in 0.1 mol/L TBAPF6 electrolyte solutions

Fig.9 Photocurrent generation with nanoSiO2BPy@(Pd/ZnTPyP)3 hybrid as light-harvesting unit in 50 mmol/L KCl solutions with(a) and without(b) 2.5 mmol/L ethyl viologen and naked ITO electrode under the same conditions(c)

Fig.10 Absorption spectra for the aqueous solution composed of the nanoSiO2BPy@(Pd/ZnTPyP)3, EV2+ and EDTA before(a) and after(b) irradiation, and spectrum after air was bubbled into the radiated solution(c)

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