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Choi, Y.,Ye, Y.,Mackeyev, Y.,Cho, M.,Lee, S.,Wilson, L.J.,Lee, J.,Alvarez, P.J.J.,Choi, W.,Lee, J. Pergamon Press ; Elsevier Science Ltd 2014 Carbon Vol.69 No.-
A magnetically recyclable photosensitizing system for harnessing solar energy for water treatment and disinfection is reported. This system comprises C<SUB>60</SUB> aminofullerene as a sensitizer for singlet oxygenation and functionalized mesoporous silica (msu-f SiO<SUB>2</SUB>) encapsulating magnetite nanoparticles (msu-SiO<SUB>2</SUB>/mag) as a magnetically separable host. Rapid degradation of furfuryl alcohol (FFA) (a singlet oxygen (<SUP>1</SUP>O<SUB>2</SUB>) probe) under visible-light irradiation along with the kinetic retardation of FFA decomposition in the presence of <SUP>1</SUP>O<SUB>2</SUB> quenchers suggests that the visible-light activity of C<SUB>60</SUB> aminofullerene-derivatized msu-SiO<SUB>2</SUB>/mag (C<SUB>60</SUB>/msu-SiO<SUB>2</SUB>/mag) is related to the photosensitization of <SUP>1</SUP>O<SUB>2</SUB>. On the other hand, the use of SiO<SUB>2</SUB> gel and fumed SiO<SUB>2</SUB> as magnetic supports drastically reduced the photosensitized generation of <SUP>1</SUP>O<SUB>2</SUB>, which is ascribed to the absence of an ordered pore structure in the alternative silica support, resulting in an uncontrolled growth of Fe<SUB>3</SUB>O<SUB>4</SUB> and an aggregation of the fullerenes on the SiO<SUB>2</SUB> gel and fumed SiO<SUB>2</SUB>. Significant <SUP>1</SUP>O<SUB>2</SUB> production using C<SUB>60</SUB>/msu-SiO<SUB>2</SUB>/mag led to the effective oxidation of emerging pharmaceutical contaminants and inactivation of MS-2 bacteriophage under visible-light irradiation. Magnetic recovery and the subsequent reuse of the composite did not cause any significant loss in the photosensitizing activity of C<SUB>60</SUB>/msu-SiO<SUB>2</SUB>/mag, demonstrating its potential for catalytic applications.
Kim, Heechan,Kim, Wooyul,Mackeyev, Yuri,Lee, Gi-Seon,Kim, Hee-Joon,Tachikawa, Takashi,Hong, Seokwon,Lee, Sanghyup,Kim, Jungbae,Wilson, Lon J.,Majima, Tetsuro,Alvarez, Pedro J. J.,Choi, Wonyong,Lee, Ja American Chemical Society 2012 Environmental science & technology Vol.46 No.17
<P>This study evaluates the potential application of tin porphyrin- and C<SUB>60</SUB> aminofullerene-derivatized silica (SnP/silica and aminoC<SUB>60</SUB>/silica) as <SUP>1</SUP>O<SUB>2</SUB> generating systems for photochemical degradation of organic pollutants. Photosensitized <SUP>1</SUP>O<SUB>2</SUB> production with SnP/silica, which was faster than with aminoC<SUB>60</SUB>/silica, effectively oxidized a variety of pharmaceuticals. Significant degradation of pharmaceuticals in the presence of the 400-nm UV cutoff filter corroborated visible light activation of both photosensitizers. Whereas the efficacy of aminoC<SUB>60</SUB>/silica for <SUP>1</SUP>O<SUB>2</SUB> production drastically decreased under irradiation with λ > 550 nm, Q-band absorption caused negligible loss of the photosensitizing activity of SnP/silica in the long wavelength region. Faster destruction of phenolates by SnP/silica and aminoC<SUB>60</SUB>/silica under alkaline pH conditions further implicated <SUP>1</SUP>O<SUB>2</SUB> involvement in the oxidative degradation. Direct charge transfer mediated by SnP, which was inferred from nanosecond laser flash photolysis, induced significant degradation of neutral phenols under high power light irradiation. Self-sensitized destruction caused gradual activity loss of SnP/silica in reuse tests unlike aminoC<SUB>60</SUB>/silica. The kinetic comparison of SnP/silica and TiO<SUB>2</SUB> photocatalyst in real wastewater effluents showed that photosensitized singlet oxygenation of pharmaceuticals was still efficiently achieved in the presence of background organic matters, while significant interference was observed for photocatalyzed oxidation involving non-selective OH radical.</P><P><B>Graphic Abstract</B> <IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/esthag/2012/esthag.2012.46.issue-17/es301775k/production/images/medium/es-2012-01775k_0009.gif'></P><P><A href='http://pubs.acs.org/doi/suppl/10.1021/es301775k'>ACS Electronic Supporting Info</A></P>
Yoo, H.Y.,Yan, S.,Ra, J.W.,Jeon, D.,Goh, B.,Kim, T.Y.,Mackeyev, Y.,Ahn, Y.Y.,Kim, H.J.,Wilson, L.J.,Alvarez, P.J.J.,Lee, Y.,Song, W.,Hong, S.W.,Kim, J.,Lee, J. Elsevier 2016 Applied catalysis. B, Environmental Vol.199 No.-
<P>This study demonstrates that tin porphyrin (SnP) loading on a silica substrate (SnP/silica) markedly accelerates the degradation of Microcystins (MCs) under visible light irradiation, despite a reduction of photosensitized singlet oxygen (O-1(2)) production. A comparative study using Rose Bengal, SnP, and C-60 aminofullerene suggested that the MC-RR decay rate was directly proportional to the photosensitizing activity for triplet state-induced oxidation, while it exhibited poor correlation to singlet oxygenation efficiency. This implies that electron transfer from MC to the triplet state of SnP (facilitated by favorable MC sorption on silica) contributes to the photosensitized MC oxidation. Experiments to examine sensitizers for the one-electron oxidation of 2,2'-azino-bis(3-ethylbenzothiazoline-6-sulfonic acid) showed the superiority of SnP/silica for photo-initiated electron transfer as a possible MC oxidation route. This was corroborated by the negligible effects of reagents that quench or facilitate singlet oxygenation (e.g., azide ion, D2O) on the MC-RR degradation rate. Despite MC-RR removal below detection levels, residual toxicity (indicated by a significant decrease in protein phosphatase inhibition activity) was observed. Tandem mass spectrometric analysis suggests that this residual toxicity may be ascribed to byproducts resulting from addition of a single oxygen atom to the Adda moiety. (C) 2016 Elsevier B.V. All rights reserved.</P>