TY - JOUR
T1 - A metal-free heptazine-porphyrin based porous polymeric network as an artificial leaf for carbon-free solar fuels
AU - Kumar, Sunil
AU - Battula, Venugopala Rao
AU - Sharma, Neha
AU - Samanta, Soumadri
AU - Rawat, Bhawna
AU - Kailasam, Kamalakannan
N1 - Funding Information:
Dr K. Kailasam thanks DST-Nano Mission NATDP funded Technology Project, File No. SR/NM/NT-06/2016 for financial support. The authors are thankful to Ms Diksha Gambhir (PhD Scholar, IIT Mandi) for her contributions during the preparation of the manuscript.
Publisher Copyright:
© 2022 The Royal Society of Chemistry.
PY - 2022/6/17
Y1 - 2022/6/17
N2 - Carbon-free solar fuel production driven by solar energy has become a holy grail for a future sustainable world. In recent years, much interest has been centered on hydrogen peroxide (H2O2), a carbon-free solar fuel that is superior to hydrogen (H2) in terms of transportation and direct use in membrane-free fuel cells. Thus, H2O2 production using solar energy from pure water over visible-light-active photocatalysts is a more sustainable approach than existing anthraquinone-based processes. Herein, for the first time, a metal-free heptazine-based porous polymeric network (HMP-PPR) featuring heptazine and porphyrin units bridged through -NH- bonds is developed. Under simulated sunlight, HMP-PPR shows nearly 9 times higher H2O2 production than graphitic carbon nitride (g-CN). Further, HMP-PPR stably generates 750 μmol g−1 H2O2 over propan-2-ol in 24 h. Interestingly, under natural sunlight, it produces 151 μmol g−1 H2O2 from pure water in 4 h through both a two-electron oxygen reduction reaction and two-electron water oxidation. Such exciting results are explained based on the unique band positions of the material, oxygraph analysis, and theoretical studies. This study explains the importance of heptazine-based porous polymeric networks in liquid solar fuel production.
AB - Carbon-free solar fuel production driven by solar energy has become a holy grail for a future sustainable world. In recent years, much interest has been centered on hydrogen peroxide (H2O2), a carbon-free solar fuel that is superior to hydrogen (H2) in terms of transportation and direct use in membrane-free fuel cells. Thus, H2O2 production using solar energy from pure water over visible-light-active photocatalysts is a more sustainable approach than existing anthraquinone-based processes. Herein, for the first time, a metal-free heptazine-based porous polymeric network (HMP-PPR) featuring heptazine and porphyrin units bridged through -NH- bonds is developed. Under simulated sunlight, HMP-PPR shows nearly 9 times higher H2O2 production than graphitic carbon nitride (g-CN). Further, HMP-PPR stably generates 750 μmol g−1 H2O2 over propan-2-ol in 24 h. Interestingly, under natural sunlight, it produces 151 μmol g−1 H2O2 from pure water in 4 h through both a two-electron oxygen reduction reaction and two-electron water oxidation. Such exciting results are explained based on the unique band positions of the material, oxygraph analysis, and theoretical studies. This study explains the importance of heptazine-based porous polymeric networks in liquid solar fuel production.
UR - http://www.scopus.com/inward/record.url?scp=85133685016&partnerID=8YFLogxK
U2 - 10.1039/d2ta01646j
DO - 10.1039/d2ta01646j
M3 - Article
AN - SCOPUS:85133685016
VL - 10
SP - 14568
EP - 14575
JO - Journal of Materials Chemistry A
JF - Journal of Materials Chemistry A
SN - 2050-7488
IS - 27
ER -
