Ultrahigh Photocatalytic Oxygen Reduction to Hydrogen Peroxide by a True Oxygen-Bridged Heptazine Polymer

Venugopala Rao Battula; Bhawna Rawat; Kamalakannan Kailasam

doi:10.1021/acsapm.2c02057

Ultrahigh Photocatalytic Oxygen Reduction to Hydrogen Peroxide by a True Oxygen-Bridged Heptazine Polymer

Venugopala Rao Battula, Bhawna Rawat, Kamalakannan Kailasam

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

2 Scopus citations

Abstract

Solar-H₂O₂ production presents an eco-friendly and sustainable strategy over the existing anthraquinone process. The present photocatalytic systems suffer from low two-electron oxygen reduction reaction (ORR) selectivity. The current study reports an easy approach to produce a true oxygen-bridged heptazine polymer with periodic arrangement of oxygen atoms (CNO) by introducing C-O-C bridging species through the right precursor selection. The C-O-C species in CNO dramatically promotes ORR compared to the benchmark carbon nitride synthesized from melamine (CNM), which has been proved by electrochemical analysis. To our surprise, the CNO has produced 1.5 mmol/g of H₂O₂ after 4 h in natural sunlight, which is the highest among the existing carbon-nitride-based photocatalysts. In addition, the challenging biomass-derived chemicals, glycerol, glucose, and 1,2-propanediol were also utilized as sacrificial electron donors in H₂O₂ production to synthesize fine chemicals. Overall, this work provides an easy approach to tune the two-electron ORR to boost H₂O₂ production and paves the way for practical solar-H₂O₂ production from biomass using polymeric O-bridged heptazines (CNO).

Original language	English
Pages (from-to)	1989-1997
Number of pages	9
Journal	ACS Applied Polymer Materials
Volume	5
Issue number	3
DOIs	https://doi.org/10.1021/acsapm.2c02057
State	Published - 10 Mar 2023
Externally published	Yes

Keywords

biomass
carbon nitride
hydrogen peroxide
solar fuels
two-electron oxygen reduction reaction

ASJC Scopus subject areas

Process Chemistry and Technology
Polymers and Plastics
Organic Chemistry

Access to Document

10.1021/acsapm.2c02057

Cite this

@article{414a96b9b6414f97b51a45f66ec0b5b4,

title = "Ultrahigh Photocatalytic Oxygen Reduction to Hydrogen Peroxide by a True Oxygen-Bridged Heptazine Polymer",

abstract = "Solar-H2O2 production presents an eco-friendly and sustainable strategy over the existing anthraquinone process. The present photocatalytic systems suffer from low two-electron oxygen reduction reaction (ORR) selectivity. The current study reports an easy approach to produce a true oxygen-bridged heptazine polymer with periodic arrangement of oxygen atoms (CNO) by introducing C-O-C bridging species through the right precursor selection. The C-O-C species in CNO dramatically promotes ORR compared to the benchmark carbon nitride synthesized from melamine (CNM), which has been proved by electrochemical analysis. To our surprise, the CNO has produced 1.5 mmol/g of H2O2 after 4 h in natural sunlight, which is the highest among the existing carbon-nitride-based photocatalysts. In addition, the challenging biomass-derived chemicals, glycerol, glucose, and 1,2-propanediol were also utilized as sacrificial electron donors in H2O2 production to synthesize fine chemicals. Overall, this work provides an easy approach to tune the two-electron ORR to boost H2O2 production and paves the way for practical solar-H2O2 production from biomass using polymeric O-bridged heptazines (CNO).",

keywords = "biomass, carbon nitride, hydrogen peroxide, solar fuels, two-electron oxygen reduction reaction",

author = "Battula, {Venugopala Rao} and Bhawna Rawat and Kamalakannan Kailasam",

note = "Funding Information: Prof. K. Kailasam thanks INST and funding agencies for the continuous support. Publisher Copyright: {\textcopyright} 2023 American Chemical Society.",

year = "2023",

month = mar,

day = "10",

doi = "10.1021/acsapm.2c02057",

language = "English",

volume = "5",

pages = "1989--1997",

journal = "ACS Applied Polymer Materials",

issn = "2637-6105",

publisher = "American Chemical Society",

number = "3",

}

TY - JOUR

T1 - Ultrahigh Photocatalytic Oxygen Reduction to Hydrogen Peroxide by a True Oxygen-Bridged Heptazine Polymer

AU - Battula, Venugopala Rao

AU - Rawat, Bhawna

AU - Kailasam, Kamalakannan

PY - 2023/3/10

Y1 - 2023/3/10

N2 - Solar-H2O2 production presents an eco-friendly and sustainable strategy over the existing anthraquinone process. The present photocatalytic systems suffer from low two-electron oxygen reduction reaction (ORR) selectivity. The current study reports an easy approach to produce a true oxygen-bridged heptazine polymer with periodic arrangement of oxygen atoms (CNO) by introducing C-O-C bridging species through the right precursor selection. The C-O-C species in CNO dramatically promotes ORR compared to the benchmark carbon nitride synthesized from melamine (CNM), which has been proved by electrochemical analysis. To our surprise, the CNO has produced 1.5 mmol/g of H2O2 after 4 h in natural sunlight, which is the highest among the existing carbon-nitride-based photocatalysts. In addition, the challenging biomass-derived chemicals, glycerol, glucose, and 1,2-propanediol were also utilized as sacrificial electron donors in H2O2 production to synthesize fine chemicals. Overall, this work provides an easy approach to tune the two-electron ORR to boost H2O2 production and paves the way for practical solar-H2O2 production from biomass using polymeric O-bridged heptazines (CNO).

AB - Solar-H2O2 production presents an eco-friendly and sustainable strategy over the existing anthraquinone process. The present photocatalytic systems suffer from low two-electron oxygen reduction reaction (ORR) selectivity. The current study reports an easy approach to produce a true oxygen-bridged heptazine polymer with periodic arrangement of oxygen atoms (CNO) by introducing C-O-C bridging species through the right precursor selection. The C-O-C species in CNO dramatically promotes ORR compared to the benchmark carbon nitride synthesized from melamine (CNM), which has been proved by electrochemical analysis. To our surprise, the CNO has produced 1.5 mmol/g of H2O2 after 4 h in natural sunlight, which is the highest among the existing carbon-nitride-based photocatalysts. In addition, the challenging biomass-derived chemicals, glycerol, glucose, and 1,2-propanediol were also utilized as sacrificial electron donors in H2O2 production to synthesize fine chemicals. Overall, this work provides an easy approach to tune the two-electron ORR to boost H2O2 production and paves the way for practical solar-H2O2 production from biomass using polymeric O-bridged heptazines (CNO).

KW - biomass

KW - carbon nitride

KW - hydrogen peroxide

KW - solar fuels

KW - two-electron oxygen reduction reaction

UR - http://www.scopus.com/inward/record.url?scp=85149112625&partnerID=8YFLogxK

U2 - 10.1021/acsapm.2c02057

DO - 10.1021/acsapm.2c02057

M3 - Article

AN - SCOPUS:85149112625

SN - 2637-6105

VL - 5

SP - 1989

EP - 1997

JO - ACS Applied Polymer Materials

JF - ACS Applied Polymer Materials

IS - 3

ER -

Ultrahigh Photocatalytic Oxygen Reduction to Hydrogen Peroxide by a True Oxygen-Bridged Heptazine Polymer

Abstract

Keywords

ASJC Scopus subject areas

Access to Document

Other files and links

Fingerprint

Cite this