Highly Active Visible Light-Promoted Ir/g-C3N4 Photocatalysts for the Water Oxidation Reaction Prepared from a Halogen-Free Iridium Precursor

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Highly Active Visible Light-Promoted Ir/g-C₃N₄ Photocatalysts for the Water Oxidation Reaction Prepared from a Halogen-Free Iridium Precursor. / Topchiyan, Polina; Vasilchenko, Danila; Tkachev, Sergey et al.

In: ACS applied materials & interfaces, Vol. 14, No. 31, 10.08.2022, p. 35600-35612.

Research output: Contribution to journal › Article › peer-review

Author

Topchiyan, Polina ; Vasilchenko, Danila ; Tkachev, Sergey et al. / Highly Active Visible Light-Promoted Ir/g-C₃N₄ Photocatalysts for the Water Oxidation Reaction Prepared from a Halogen-Free Iridium Precursor. In: ACS applied materials & interfaces. 2022 ; Vol. 14, No. 31. pp. 35600-35612.

BibTeX

@article{772727836c66485d97bc1ae62566e9a3,

title = "Highly Active Visible Light-Promoted Ir/g-C3N4 Photocatalysts for the Water Oxidation Reaction Prepared from a Halogen-Free Iridium Precursor",

abstract = "A combination of the exceptional stability of fac-[Ir(H2O)3(NO2)3] together with thermolability of nitro and aqua ligands and high solubility in various solvents makes it promising as a brand-new chlorine-free precursor of iridium for the preparation of heterogeneous catalysts. In the current work, a new technique of fac-[Ir(H2O)3(NO2)3] preparation based on hydrothermal treatment of (NH4)3[Ir(NO2)6] was developed. For this purpose, the influence of reaction parameters such as the reaction time, temperature, and pH of the solution on the process of hexanitroiridate salt hydrolysis was investigated. The synthesized fac-[Ir(H2O)3(NO2)3] solution in this optimized way was used for the preparation of the series of Ir/g-C3N4 catalysts, which were evaluated in the water oxidation reaction with NaIO4 utilized as a sacrificial reagent. A 20-fold enhancement of the oxygen evolution reaction (OER) activity was found to take place under visible light (λ = 411 nm) illumination of the systems. The highest rate of the photoinduced OER per iridium center was achieved by the Ir0.005/g-C3N4 (air, 400°C) catalyst with an exceptional turnover frequency value of 967 min-1 approaching the activity of known homogeneous iridium OER catalysts. The leaching experiments have shown that aquated Ir species are generated in a solution after prolonged functioning of the catalysts. Despite this, in the closed system the photodriven OER activity persists at a steady-state level evidencing an equilibrium achieved between dissolved and anchored Ir species forming catalytic tandem with the g-C3N4.",

keywords = "g-C3N4, iridium, oxygen evolution reaction, photocatalyst, visible light, g-C N",

author = "Polina Topchiyan and Danila Vasilchenko and Sergey Tkachev and Dmitriy Sheven and Ilia Eltsov and Igor Asanov and Nikolay Sidorenko and Andrey Saraev and Evgeny Gerasimov and Anna Kurenkova and Ekaterina Kozlova",

note = "Funding Information: This work was supported by the Russian Science Foundation (RSF grant 21-13-00314). The authors deeply thank XRD Facility of NIIC SB RAS for the single-crystal data collection, Dr. Plyusnin P.E for thermogravimetric analysis, and Yushina I.V. for DRS analysis. Publisher Copyright: {\textcopyright} 2022 American Chemical Society.",

year = "2022",

month = aug,

day = "10",

doi = "10.1021/acsami.2c07485",

language = "English",

volume = "14",

pages = "35600--35612",

journal = "ACS applied materials & interfaces",

issn = "1944-8244",

publisher = "American Chemical Society",

number = "31",

}

RIS

TY - JOUR

T1 - Highly Active Visible Light-Promoted Ir/g-C3N4 Photocatalysts for the Water Oxidation Reaction Prepared from a Halogen-Free Iridium Precursor

AU - Topchiyan, Polina

AU - Vasilchenko, Danila

AU - Tkachev, Sergey

AU - Sheven, Dmitriy

AU - Eltsov, Ilia

AU - Asanov, Igor

AU - Sidorenko, Nikolay

AU - Saraev, Andrey

AU - Gerasimov, Evgeny

AU - Kurenkova, Anna

AU - Kozlova, Ekaterina

N1 - Funding Information: This work was supported by the Russian Science Foundation (RSF grant 21-13-00314). The authors deeply thank XRD Facility of NIIC SB RAS for the single-crystal data collection, Dr. Plyusnin P.E for thermogravimetric analysis, and Yushina I.V. for DRS analysis. Publisher Copyright: © 2022 American Chemical Society.

PY - 2022/8/10

Y1 - 2022/8/10

N2 - A combination of the exceptional stability of fac-[Ir(H2O)3(NO2)3] together with thermolability of nitro and aqua ligands and high solubility in various solvents makes it promising as a brand-new chlorine-free precursor of iridium for the preparation of heterogeneous catalysts. In the current work, a new technique of fac-[Ir(H2O)3(NO2)3] preparation based on hydrothermal treatment of (NH4)3[Ir(NO2)6] was developed. For this purpose, the influence of reaction parameters such as the reaction time, temperature, and pH of the solution on the process of hexanitroiridate salt hydrolysis was investigated. The synthesized fac-[Ir(H2O)3(NO2)3] solution in this optimized way was used for the preparation of the series of Ir/g-C3N4 catalysts, which were evaluated in the water oxidation reaction with NaIO4 utilized as a sacrificial reagent. A 20-fold enhancement of the oxygen evolution reaction (OER) activity was found to take place under visible light (λ = 411 nm) illumination of the systems. The highest rate of the photoinduced OER per iridium center was achieved by the Ir0.005/g-C3N4 (air, 400°C) catalyst with an exceptional turnover frequency value of 967 min-1 approaching the activity of known homogeneous iridium OER catalysts. The leaching experiments have shown that aquated Ir species are generated in a solution after prolonged functioning of the catalysts. Despite this, in the closed system the photodriven OER activity persists at a steady-state level evidencing an equilibrium achieved between dissolved and anchored Ir species forming catalytic tandem with the g-C3N4.

AB - A combination of the exceptional stability of fac-[Ir(H2O)3(NO2)3] together with thermolability of nitro and aqua ligands and high solubility in various solvents makes it promising as a brand-new chlorine-free precursor of iridium for the preparation of heterogeneous catalysts. In the current work, a new technique of fac-[Ir(H2O)3(NO2)3] preparation based on hydrothermal treatment of (NH4)3[Ir(NO2)6] was developed. For this purpose, the influence of reaction parameters such as the reaction time, temperature, and pH of the solution on the process of hexanitroiridate salt hydrolysis was investigated. The synthesized fac-[Ir(H2O)3(NO2)3] solution in this optimized way was used for the preparation of the series of Ir/g-C3N4 catalysts, which were evaluated in the water oxidation reaction with NaIO4 utilized as a sacrificial reagent. A 20-fold enhancement of the oxygen evolution reaction (OER) activity was found to take place under visible light (λ = 411 nm) illumination of the systems. The highest rate of the photoinduced OER per iridium center was achieved by the Ir0.005/g-C3N4 (air, 400°C) catalyst with an exceptional turnover frequency value of 967 min-1 approaching the activity of known homogeneous iridium OER catalysts. The leaching experiments have shown that aquated Ir species are generated in a solution after prolonged functioning of the catalysts. Despite this, in the closed system the photodriven OER activity persists at a steady-state level evidencing an equilibrium achieved between dissolved and anchored Ir species forming catalytic tandem with the g-C3N4.

KW - g-C3N4

KW - iridium

KW - oxygen evolution reaction

KW - photocatalyst

KW - visible light

KW - g-C N

UR - http://www.scopus.com/inward/record.url?scp=85135768520&partnerID=8YFLogxK

U2 - 10.1021/acsami.2c07485

DO - 10.1021/acsami.2c07485

M3 - Article

C2 - 35881890

AN - SCOPUS:85135768520

VL - 14

SP - 35600

EP - 35612

JO - ACS applied materials & interfaces

JF - ACS applied materials & interfaces

SN - 1944-8244

IS - 31

ER -

ID: 36844139