Bottom-up and top-down methods to improve catalytic reactivity for photocatalytic production of hydrogen peroxide using a Ru-complex and water oxidation catalystsElectronic supplementary information (ESI) available: Experimental section, time courses of H2O2 production under different conditions (Fig. S1, S2, S14-S17), TEM images (Fig. S3, S5 and S13), X-ray photoelectron spectra of Ir(OH)3 (Fig. S4), time course of H2O2 decomposition in the presence of NiFe2O4 (Fig. S6), DLS data (Fig. S7-S10),

Hydrogen peroxide (H 2 O 2 ) was produced from water and dioxygen using [Ru II (Me 2 phen) 3 ] 2+ (Me 2 phen = 4,7-dimethyl-1,10-phenanthroline) as a photocatalyst and [Ir(Cp*)(H 2 O) 3 ] 2+ (Cp* = η 5 -pentamethylcyclopentadienyl) as a precursor of a water oxidation catalyst in the presence of Sc 3...

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Main Authors Isaka, Yusuke, Kato, Satoshi, Hong, Dachao, Suenobu, Tomoyoshi, Yamada, Yusuke, Fukuzumi, Shunichi
Format Journal Article
LanguageEnglish
Published 02.06.2015
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Abstract Hydrogen peroxide (H 2 O 2 ) was produced from water and dioxygen using [Ru II (Me 2 phen) 3 ] 2+ (Me 2 phen = 4,7-dimethyl-1,10-phenanthroline) as a photocatalyst and [Ir(Cp*)(H 2 O) 3 ] 2+ (Cp* = η 5 -pentamethylcyclopentadienyl) as a precursor of a water oxidation catalyst in the presence of Sc 3+ in water under visible light irradiation. TEM and XPS measurements of residues in the resulting solution after the photocatalytic production of H 2 O 2 indicated that [Ir(Cp*)(H 2 O) 3 ] 2+ was converted to Ir(OH) 3 nanoparticles, which are actual catalytic species. The Ir(OH) 3 nanoparticles produced in situ during the photocatalytic production of H 2 O 2 were smaller in size than those prepared independently from hydrogen hexachloroiridiate (H 2 IrCl 6 ), and exhibited higher catalytic reactivity for the photocatalytic production of H 2 O 2 . The photocatalytic production of H 2 O 2 from water and dioxygen was also made possible when Ir(OH) 3 nanoparticles were replaced by nickel ferrite (NiFe 2 O 4 ) nanoparticles, which are composed of more earth abundant metals than iridium. The size of NiFe 2 O 4 nanoparticles became smaller during the photocatalytic production of H 2 O 2 to exhibit higher catalytic reactivity in the second run as compared with that in the first run. NiFe 2 O 4 nanoparticles obtained by the treatment of NiFe 2 O 4 in an aqueous solution of Sc 3+ exhibited 33-times higher catalytic reactivity in H 2 O 2 -production rates than the as-prepared NiFe 2 O 4 . Thus, both the bottom-up method starting from a molecular complex [Ir(Cp*)(H 2 O) 3 ] 2+ and the top-down method starting from as-prepared NiFe 2 O 4 to obtain nanoparticles with smaller size resulted in the improvement of the catalytic reactivity for the photocatalytic production of H 2 O 2 from water and dioxygen. Hydrogen peroxide (H 2 O 2 ) was produced from water and dioxygen using a Ru-complex photocatalyst and water oxidation catalysts of metal-containing nanoparticles produced in situ under visible light irradiation.
AbstractList Hydrogen peroxide (H 2 O 2 ) was produced from water and dioxygen using [Ru II (Me 2 phen) 3 ] 2+ (Me 2 phen = 4,7-dimethyl-1,10-phenanthroline) as a photocatalyst and [Ir(Cp*)(H 2 O) 3 ] 2+ (Cp* = η 5 -pentamethylcyclopentadienyl) as a precursor of a water oxidation catalyst in the presence of Sc 3+ in water under visible light irradiation. TEM and XPS measurements of residues in the resulting solution after the photocatalytic production of H 2 O 2 indicated that [Ir(Cp*)(H 2 O) 3 ] 2+ was converted to Ir(OH) 3 nanoparticles, which are actual catalytic species. The Ir(OH) 3 nanoparticles produced in situ during the photocatalytic production of H 2 O 2 were smaller in size than those prepared independently from hydrogen hexachloroiridiate (H 2 IrCl 6 ), and exhibited higher catalytic reactivity for the photocatalytic production of H 2 O 2 . The photocatalytic production of H 2 O 2 from water and dioxygen was also made possible when Ir(OH) 3 nanoparticles were replaced by nickel ferrite (NiFe 2 O 4 ) nanoparticles, which are composed of more earth abundant metals than iridium. The size of NiFe 2 O 4 nanoparticles became smaller during the photocatalytic production of H 2 O 2 to exhibit higher catalytic reactivity in the second run as compared with that in the first run. NiFe 2 O 4 nanoparticles obtained by the treatment of NiFe 2 O 4 in an aqueous solution of Sc 3+ exhibited 33-times higher catalytic reactivity in H 2 O 2 -production rates than the as-prepared NiFe 2 O 4 . Thus, both the bottom-up method starting from a molecular complex [Ir(Cp*)(H 2 O) 3 ] 2+ and the top-down method starting from as-prepared NiFe 2 O 4 to obtain nanoparticles with smaller size resulted in the improvement of the catalytic reactivity for the photocatalytic production of H 2 O 2 from water and dioxygen. Hydrogen peroxide (H 2 O 2 ) was produced from water and dioxygen using a Ru-complex photocatalyst and water oxidation catalysts of metal-containing nanoparticles produced in situ under visible light irradiation.
Author Kato, Satoshi
Hong, Dachao
Isaka, Yusuke
Fukuzumi, Shunichi
Yamada, Yusuke
Suenobu, Tomoyoshi
AuthorAffiliation Ewha Womans University
Department of Bioinspired Science
Japan Science and Technology Agency (JST)
SENTAN
ALCA
Department of Material and Life Science
Meijo University
Osaka University
Faculty of Science and Engineering
Graduate School of Engineering
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Notes decomposition in the presence of NiFe
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10.1039/c5ta02446c
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(Fig. S4), time course of H
Electronic supplementary information (ESI) available: Experimental section, time courses of H
(Fig. S6), DLS data (Fig. S7-S10), powder XRD patterns (Fig. S11), UV-Vis spectra (Fig. S12) and appendix for the derivation of specific surface area of particles. See DOI
O
production under different conditions (Fig. S1, S2, S14-S17), TEM images (Fig. S3, S5 and S13), X-ray photoelectron spectra of Ir(OH)
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  publication-title: Hydrogen as a Future Energy Carrier
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Title Bottom-up and top-down methods to improve catalytic reactivity for photocatalytic production of hydrogen peroxide using a Ru-complex and water oxidation catalystsElectronic supplementary information (ESI) available: Experimental section, time courses of H2O2 production under different conditions (Fig. S1, S2, S14-S17), TEM images (Fig. S3, S5 and S13), X-ray photoelectron spectra of Ir(OH)3 (Fig. S4), time course of H2O2 decomposition in the presence of NiFe2O4 (Fig. S6), DLS data (Fig. S7-S10),
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