Synergistic Enhancement of H 2 and CH 4 Evolution by CO 2 Photoreduction in Water with Reduced Graphene Oxide-Bismuth Monoxide Quantum Dot Catalyst

Research output: Contribution to journalArticle

Abstract

Photocatalytic water splitting or CO 2 reduction is one of the most promising strategies for solar energy conversion into hydrogen-containing fuels. However, these two processes typically compete with each other, which significantly decreases the solar energy conversion efficiency. Herein, we report for the first time this competition can be overcome by modulation of reactive sites and electron transfer pathway of heterogeneous photocatalysts. As a prototype, BiO composite reduced graphene oxide quantum dots (RGO-BiO QDs) were synthesized, which can provide large amounts of photogenerated electrons as well as individual reactive sites for H + and CO 2 reduction. The productivity of H 2 , CH 4 , and CO by the RGO-BiO QDs catalyst were 102.5, 21.75, and 4.5 μmol/(g·h), respectively, in pure water without the assistance of any cocatalyst or sacrificial agent. The apparent quantum efficiency at 300 nm reached to 4.2%, which is more than 10 times higher than that of RGO-TiO 2 QDs (0.28%) under the same conditions. In situ DRIFT, ESR, and photoelectrochemical studies confirmed that the unique circled electron transfer pathway (E vb (BiO) → E cb (BiO) → E f (RGO) → E Vo• (BiO)) and the large amount of separated different reactive sites are responsible for the highly efficient simultaneous H 2 evolution and CO 2 reduction performance.

Original languageEnglish
Pages (from-to)2104-2112
Number of pages9
JournalACS Applied Energy Materials
Volume2
Issue number3
DOIs
Publication statusPublished - Mar 25 2019

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Carbon Monoxide
Bismuth
Graphene
Semiconductor quantum dots
Energy conversion
Solar energy
Catalysts
Oxides
Electrons
Water
Photocatalysts
Quantum efficiency
Conversion efficiency
Paramagnetic resonance
Productivity
Modulation
Hydrogen
Composite materials
bismuth oxide

All Science Journal Classification (ASJC) codes

  • Energy Engineering and Power Technology
  • Chemical Engineering (miscellaneous)
  • Electrochemistry
  • Materials Chemistry
  • Electrical and Electronic Engineering

Cite this

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title = "Synergistic Enhancement of H 2 and CH 4 Evolution by CO 2 Photoreduction in Water with Reduced Graphene Oxide-Bismuth Monoxide Quantum Dot Catalyst",
abstract = "Photocatalytic water splitting or CO 2 reduction is one of the most promising strategies for solar energy conversion into hydrogen-containing fuels. However, these two processes typically compete with each other, which significantly decreases the solar energy conversion efficiency. Herein, we report for the first time this competition can be overcome by modulation of reactive sites and electron transfer pathway of heterogeneous photocatalysts. As a prototype, BiO composite reduced graphene oxide quantum dots (RGO-BiO QDs) were synthesized, which can provide large amounts of photogenerated electrons as well as individual reactive sites for H + and CO 2 reduction. The productivity of H 2 , CH 4 , and CO by the RGO-BiO QDs catalyst were 102.5, 21.75, and 4.5 μmol/(g·h), respectively, in pure water without the assistance of any cocatalyst or sacrificial agent. The apparent quantum efficiency at 300 nm reached to 4.2{\%}, which is more than 10 times higher than that of RGO-TiO 2 QDs (0.28{\%}) under the same conditions. In situ DRIFT, ESR, and photoelectrochemical studies confirmed that the unique circled electron transfer pathway (E vb (BiO) → E cb (BiO) → E f (RGO) → E Vo• (BiO)) and the large amount of separated different reactive sites are responsible for the highly efficient simultaneous H 2 evolution and CO 2 reduction performance.",
author = "Songmei Sun and Motonori Watanabe and Pangpang Wang and Tatsumi Ishihara",
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T1 - Synergistic Enhancement of H 2 and CH 4 Evolution by CO 2 Photoreduction in Water with Reduced Graphene Oxide-Bismuth Monoxide Quantum Dot Catalyst

AU - Sun, Songmei

AU - Watanabe, Motonori

AU - Wang, Pangpang

AU - Ishihara, Tatsumi

PY - 2019/3/25

Y1 - 2019/3/25

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AB - Photocatalytic water splitting or CO 2 reduction is one of the most promising strategies for solar energy conversion into hydrogen-containing fuels. However, these two processes typically compete with each other, which significantly decreases the solar energy conversion efficiency. Herein, we report for the first time this competition can be overcome by modulation of reactive sites and electron transfer pathway of heterogeneous photocatalysts. As a prototype, BiO composite reduced graphene oxide quantum dots (RGO-BiO QDs) were synthesized, which can provide large amounts of photogenerated electrons as well as individual reactive sites for H + and CO 2 reduction. The productivity of H 2 , CH 4 , and CO by the RGO-BiO QDs catalyst were 102.5, 21.75, and 4.5 μmol/(g·h), respectively, in pure water without the assistance of any cocatalyst or sacrificial agent. The apparent quantum efficiency at 300 nm reached to 4.2%, which is more than 10 times higher than that of RGO-TiO 2 QDs (0.28%) under the same conditions. In situ DRIFT, ESR, and photoelectrochemical studies confirmed that the unique circled electron transfer pathway (E vb (BiO) → E cb (BiO) → E f (RGO) → E Vo• (BiO)) and the large amount of separated different reactive sites are responsible for the highly efficient simultaneous H 2 evolution and CO 2 reduction performance.

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