Photocatalytic hydrogen peroxide production by anthraquinone-augmented polymeric carbon nitride

Hyoung il Kim, Yeoseon Choi, Shu Hu, Wonyong Choi, Jae Hong Kim

Research output: Contribution to journalArticle

27 Citations (Scopus)

Abstract

We describe the exploitation of the selective catalytic property of anthraquinone (AQ) for solar photocatalytic synthesis of hydrogen peroxide (H2O2) as a green, sustainable alternative to organic-solvent-based and energy-intensive industry-benchmark processes that also rely on AQ catalysis. We accomplished this by anchoring AQ onto polymeric carbon nitride (C3N4), a metal-free visible light photocatalyst (band gap energy = 2.7 eV), that has been previously demonstrated for selective H2O2 synthesis. A net H2O2 production rate of 361 μmol g−1 h−1 and an apparent quantum yield (AQY) of 19.5% at 380 nm excitation were achieved using AQ-augmented C3N4 under simulated 1-sun illumination in the presence of an organic electron donor (2-propanol); these results were 4.4-fold and 8.3-fold higher than those reported for bare C3N4, respectively. A suite of experimental analyses confirmed the unique roles of AQ co-catalysis in (i) capturing electrons from the conduction band of C3N4, thereby reducing futile exciton recombination, which is otherwise prevalent in bare C3N4; (ii) effectively mediating electron transfer to drive hydrogenation reaction to form anthrahydroquinone (AQH2) from AQ; and (iii) catalyzing oxygen reduction to H2O2 through the dehydrogenation of AQH2 back to AQ, resulting in the facile and selective formation of H2O2. In addition, the reduced decomposition of produced H2O2 by the C3N4/AQ composite photocatalysts, when compared to bare C3N4 or C3N4 composited with common metallic co-catalysts such as Pt and Ag, was found to contribute to the significant enhancement in H2O2 production through the oxidation of both organic and water.

Original languageEnglish
Pages (from-to)121-129
Number of pages9
JournalApplied Catalysis B: Environmental
Volume229
DOIs
Publication statusPublished - 2018 Aug 5

Fingerprint

Anthraquinones
Carbon nitride
Hydrogen peroxide
hydrogen peroxide
Hydrogen Peroxide
catalysis
Photocatalysts
electron
Catalysis
Electrons
carbon
fold
Propanol
Quantum yield
Dehydrogenation
Conduction bands
Excitons
Sun
Organic solvents
recombination

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Environmental Science(all)
  • Process Chemistry and Technology

Cite this

Kim, Hyoung il ; Choi, Yeoseon ; Hu, Shu ; Choi, Wonyong ; Kim, Jae Hong. / Photocatalytic hydrogen peroxide production by anthraquinone-augmented polymeric carbon nitride. In: Applied Catalysis B: Environmental. 2018 ; Vol. 229. pp. 121-129.
@article{1cad05ed678d4f8cb17a29f4ac292e12,
title = "Photocatalytic hydrogen peroxide production by anthraquinone-augmented polymeric carbon nitride",
abstract = "We describe the exploitation of the selective catalytic property of anthraquinone (AQ) for solar photocatalytic synthesis of hydrogen peroxide (H2O2) as a green, sustainable alternative to organic-solvent-based and energy-intensive industry-benchmark processes that also rely on AQ catalysis. We accomplished this by anchoring AQ onto polymeric carbon nitride (C3N4), a metal-free visible light photocatalyst (band gap energy = 2.7 eV), that has been previously demonstrated for selective H2O2 synthesis. A net H2O2 production rate of 361 μmol g−1 h−1 and an apparent quantum yield (AQY) of 19.5{\%} at 380 nm excitation were achieved using AQ-augmented C3N4 under simulated 1-sun illumination in the presence of an organic electron donor (2-propanol); these results were 4.4-fold and 8.3-fold higher than those reported for bare C3N4, respectively. A suite of experimental analyses confirmed the unique roles of AQ co-catalysis in (i) capturing electrons from the conduction band of C3N4, thereby reducing futile exciton recombination, which is otherwise prevalent in bare C3N4; (ii) effectively mediating electron transfer to drive hydrogenation reaction to form anthrahydroquinone (AQH2) from AQ; and (iii) catalyzing oxygen reduction to H2O2 through the dehydrogenation of AQH2 back to AQ, resulting in the facile and selective formation of H2O2. In addition, the reduced decomposition of produced H2O2 by the C3N4/AQ composite photocatalysts, when compared to bare C3N4 or C3N4 composited with common metallic co-catalysts such as Pt and Ag, was found to contribute to the significant enhancement in H2O2 production through the oxidation of both organic and water.",
author = "Kim, {Hyoung il} and Yeoseon Choi and Shu Hu and Wonyong Choi and Kim, {Jae Hong}",
year = "2018",
month = "8",
day = "5",
doi = "10.1016/j.apcatb.2018.01.060",
language = "English",
volume = "229",
pages = "121--129",
journal = "Applied Catalysis B: Environmental",
issn = "0926-3373",
publisher = "Elsevier",

}

Photocatalytic hydrogen peroxide production by anthraquinone-augmented polymeric carbon nitride. / Kim, Hyoung il; Choi, Yeoseon; Hu, Shu; Choi, Wonyong; Kim, Jae Hong.

In: Applied Catalysis B: Environmental, Vol. 229, 05.08.2018, p. 121-129.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Photocatalytic hydrogen peroxide production by anthraquinone-augmented polymeric carbon nitride

AU - Kim, Hyoung il

AU - Choi, Yeoseon

AU - Hu, Shu

AU - Choi, Wonyong

AU - Kim, Jae Hong

PY - 2018/8/5

Y1 - 2018/8/5

N2 - We describe the exploitation of the selective catalytic property of anthraquinone (AQ) for solar photocatalytic synthesis of hydrogen peroxide (H2O2) as a green, sustainable alternative to organic-solvent-based and energy-intensive industry-benchmark processes that also rely on AQ catalysis. We accomplished this by anchoring AQ onto polymeric carbon nitride (C3N4), a metal-free visible light photocatalyst (band gap energy = 2.7 eV), that has been previously demonstrated for selective H2O2 synthesis. A net H2O2 production rate of 361 μmol g−1 h−1 and an apparent quantum yield (AQY) of 19.5% at 380 nm excitation were achieved using AQ-augmented C3N4 under simulated 1-sun illumination in the presence of an organic electron donor (2-propanol); these results were 4.4-fold and 8.3-fold higher than those reported for bare C3N4, respectively. A suite of experimental analyses confirmed the unique roles of AQ co-catalysis in (i) capturing electrons from the conduction band of C3N4, thereby reducing futile exciton recombination, which is otherwise prevalent in bare C3N4; (ii) effectively mediating electron transfer to drive hydrogenation reaction to form anthrahydroquinone (AQH2) from AQ; and (iii) catalyzing oxygen reduction to H2O2 through the dehydrogenation of AQH2 back to AQ, resulting in the facile and selective formation of H2O2. In addition, the reduced decomposition of produced H2O2 by the C3N4/AQ composite photocatalysts, when compared to bare C3N4 or C3N4 composited with common metallic co-catalysts such as Pt and Ag, was found to contribute to the significant enhancement in H2O2 production through the oxidation of both organic and water.

AB - We describe the exploitation of the selective catalytic property of anthraquinone (AQ) for solar photocatalytic synthesis of hydrogen peroxide (H2O2) as a green, sustainable alternative to organic-solvent-based and energy-intensive industry-benchmark processes that also rely on AQ catalysis. We accomplished this by anchoring AQ onto polymeric carbon nitride (C3N4), a metal-free visible light photocatalyst (band gap energy = 2.7 eV), that has been previously demonstrated for selective H2O2 synthesis. A net H2O2 production rate of 361 μmol g−1 h−1 and an apparent quantum yield (AQY) of 19.5% at 380 nm excitation were achieved using AQ-augmented C3N4 under simulated 1-sun illumination in the presence of an organic electron donor (2-propanol); these results were 4.4-fold and 8.3-fold higher than those reported for bare C3N4, respectively. A suite of experimental analyses confirmed the unique roles of AQ co-catalysis in (i) capturing electrons from the conduction band of C3N4, thereby reducing futile exciton recombination, which is otherwise prevalent in bare C3N4; (ii) effectively mediating electron transfer to drive hydrogenation reaction to form anthrahydroquinone (AQH2) from AQ; and (iii) catalyzing oxygen reduction to H2O2 through the dehydrogenation of AQH2 back to AQ, resulting in the facile and selective formation of H2O2. In addition, the reduced decomposition of produced H2O2 by the C3N4/AQ composite photocatalysts, when compared to bare C3N4 or C3N4 composited with common metallic co-catalysts such as Pt and Ag, was found to contribute to the significant enhancement in H2O2 production through the oxidation of both organic and water.

UR - http://www.scopus.com/inward/record.url?scp=85042201510&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85042201510&partnerID=8YFLogxK

U2 - 10.1016/j.apcatb.2018.01.060

DO - 10.1016/j.apcatb.2018.01.060

M3 - Article

AN - SCOPUS:85042201510

VL - 229

SP - 121

EP - 129

JO - Applied Catalysis B: Environmental

JF - Applied Catalysis B: Environmental

SN - 0926-3373

ER -