Oxygen doping and hollow structure-mediated effects to enable rapid electron transfer during photocatalytic hydrogen peroxide production

The photocatalytic production of hydrogen peroxide using solar energy is an environment-friendly solution to the energy crisis, but its low efficiency hinders its scale-up feasibility. In this work, a hollow core-shell structure OCN@In 2 S 3 composite photocatalyst was constructed by growing In 2 S...

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Veröffentlicht in:Science China materials 2024, Vol.67 (1), p.153-161
Hauptverfasser: Xu, Yandong, Tai, Wanyu, Wang, Zhirui, Zhang, Linlin, Wang, Dexin, Liao, Jianjun
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container_issue 1
container_start_page 153
container_title Science China materials
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creator Xu, Yandong
Tai, Wanyu
Wang, Zhirui
Zhang, Linlin
Wang, Dexin
Liao, Jianjun
description The photocatalytic production of hydrogen peroxide using solar energy is an environment-friendly solution to the energy crisis, but its low efficiency hinders its scale-up feasibility. In this work, a hollow core-shell structure OCN@In 2 S 3 composite photocatalyst was constructed by growing In 2 S 3 ultrathin nanosheets on the surface of O-doped hollow g-C 3 N 4 nanospheres using a two-step hydrothermal method. The hollow structure provided a high specific surface area and enhanced light absorption. O doping increased the number of active sites, and the heterojunction promoted the rapid separation and transfer of photogenerated carriers. Under visible light irradiation, the H 2 O 2 yield of OCN@In 2 S 3 reached 632.5 µmol h −1 g −1 , which was 5.7 times higher than that of g-C 3 N 4 and 12.3 times that of In 2 S 3 , as well as higher than most g-C 3 N 4 -based photocatalysts. Quenching experiments and electron paramagnetic resonance spectroscopy showed that ·O 2 − was an intermediate product formed during photocatalytic H 2 O 2 generation. The reaction primarily followed a two-step single-electron pathway. The Koutecky-Levich diagram confirmed that the synthesized OCN@In 2 S 3 maintained a high two-electron ORR selectivity during the catalytic reaction ( n = 1.67). The photocatalytic mechanism was elucidated by photoluminescence, electrochemical impedance spectroscopy, and ultraviolet photoelectron spectro-scopy, which confirmed that OCN@In 2 S 3 inhibited the recombination of photogenerated carriers. This work provides a simple and attractive strategy for developing highly active energy-conversion photocatalysts.
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In this work, a hollow core-shell structure OCN@In 2 S 3 composite photocatalyst was constructed by growing In 2 S 3 ultrathin nanosheets on the surface of O-doped hollow g-C 3 N 4 nanospheres using a two-step hydrothermal method. The hollow structure provided a high specific surface area and enhanced light absorption. O doping increased the number of active sites, and the heterojunction promoted the rapid separation and transfer of photogenerated carriers. Under visible light irradiation, the H 2 O 2 yield of OCN@In 2 S 3 reached 632.5 µmol h −1 g −1 , which was 5.7 times higher than that of g-C 3 N 4 and 12.3 times that of In 2 S 3 , as well as higher than most g-C 3 N 4 -based photocatalysts. Quenching experiments and electron paramagnetic resonance spectroscopy showed that ·O 2 − was an intermediate product formed during photocatalytic H 2 O 2 generation. The reaction primarily followed a two-step single-electron pathway. The Koutecky-Levich diagram confirmed that the synthesized OCN@In 2 S 3 maintained a high two-electron ORR selectivity during the catalytic reaction ( n = 1.67). The photocatalytic mechanism was elucidated by photoluminescence, electrochemical impedance spectroscopy, and ultraviolet photoelectron spectro-scopy, which confirmed that OCN@In 2 S 3 inhibited the recombination of photogenerated carriers. 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China Mater</addtitle><description>The photocatalytic production of hydrogen peroxide using solar energy is an environment-friendly solution to the energy crisis, but its low efficiency hinders its scale-up feasibility. In this work, a hollow core-shell structure OCN@In 2 S 3 composite photocatalyst was constructed by growing In 2 S 3 ultrathin nanosheets on the surface of O-doped hollow g-C 3 N 4 nanospheres using a two-step hydrothermal method. The hollow structure provided a high specific surface area and enhanced light absorption. O doping increased the number of active sites, and the heterojunction promoted the rapid separation and transfer of photogenerated carriers. Under visible light irradiation, the H 2 O 2 yield of OCN@In 2 S 3 reached 632.5 µmol h −1 g −1 , which was 5.7 times higher than that of g-C 3 N 4 and 12.3 times that of In 2 S 3 , as well as higher than most g-C 3 N 4 -based photocatalysts. Quenching experiments and electron paramagnetic resonance spectroscopy showed that ·O 2 − was an intermediate product formed during photocatalytic H 2 O 2 generation. The reaction primarily followed a two-step single-electron pathway. The Koutecky-Levich diagram confirmed that the synthesized OCN@In 2 S 3 maintained a high two-electron ORR selectivity during the catalytic reaction ( n = 1.67). The photocatalytic mechanism was elucidated by photoluminescence, electrochemical impedance spectroscopy, and ultraviolet photoelectron spectro-scopy, which confirmed that OCN@In 2 S 3 inhibited the recombination of photogenerated carriers. 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subjects Carbon nitride
Chemistry and Materials Science
Chemistry/Food Science
Core-shell structure
Doping
Electrochemical impedance spectroscopy
Electromagnetic absorption
Electron paramagnetic resonance
Electron transfer
Energy conversion
Heterojunctions
Hydrogen peroxide
Hydrogen production
Light irradiation
Materials Science
Nanospheres
Photocatalysis
Photocatalysts
Photoelectrons
Photoluminescence
Single electrons
Solar energy
Spectrum analysis
title Oxygen doping and hollow structure-mediated effects to enable rapid electron transfer during photocatalytic hydrogen peroxide production
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