Heteroatom Dopants Promote Two‐Electron O2 Reduction for Photocatalytic Production of H2O2 on Polymeric Carbon Nitride
- 20 May 2020
- journal article
- research article
- Published by Wiley in Angewandte Chemie
- Vol. 59 (37), 16209-16217
- https://doi.org/10.1002/anie.202006747
Abstract
Polymeric carbon nitride modified with selected heteroatom dopants in a cyclic melon was prepared and used as a model photocatalyst to identify and understand the key mechanisms required for efficient photoproduction of H 2 O 2 via selective oxygen reduction reaction (ORR). The photochemical production of H 2 O 2 was achieved at a millimolar level per hour under visible light irradiation along with 100% apparent quantum yield (in 360‐450 nm region) and 96% selectivity in an electrochemical system (0.1 V vs. RHE). Spectroscopic analysis in spatiotemporal resolution and theoretical calculations revealed that the synergistic association of alkali and sulfur dopants in polymeric matrix promoted the interlayer charge separation and polarization of trapped electrons for preferable oxygen capture and reduction in ORR kinetics. This work highlights the key features that are responsible for controlling the photocatalytic activity and selectivity toward the two‐electron ORR, which should be the basis of further development of solar H 2 O 2 production.Keywords
This publication has 72 references indexed in Scilit:
- Hydrogen peroxide as a sustainable energy carrier: Electrocatalytic production of hydrogen peroxide and the fuel cellElectrochimica Acta, 2012
- Photocatalytic H2O2 Production from Ethanol/O2 System Using TiO2 Loaded with Au–Ag Bimetallic Alloy NanoparticlesACS Catalysis, 2012
- Nanoporous Graphitic-C3N4@Carbon Metal-Free Electrocatalysts for Highly Efficient Oxygen ReductionJournal of the American Chemical Society, 2011
- In Situ Liquid Phase Synthesis of Hydrogen Peroxide from Molecular Oxygen Using Gold Nanoparticle-Loaded Titanium(IV) Dioxide PhotocatalystJournal of the American Chemical Society, 2010
- New directions in carbonitride research: synthesis of resin-like dense-packed C3N4 using a hydrogen-free precursorJournal of Materials Chemistry, 2010
- Switching Off Hydrogen Peroxide Hydrogenation in the Direct Synthesis ProcessScience, 2009
- Hydrogen Peroxide Synthesis: An Outlook beyond the Anthraquinone ProcessAngewandte Chemie, 2006
- Wasserstoffperoxid‐Synthese: Perspektiven jenseits des Anthrachinon‐VerfahrensAngewandte Chemie, 2006
- The direct formation of H2O2 from H2 and O2 over palladium catalystsJournal of Catalysis, 2003
- Oxygen Reduction on Platinum Low-Index Single-Crystal Surfaces in Sulfuric Acid Solution: Rotating Ring-Pt(hkl) Disk StudiesThe Journal of Physical Chemistry, 1995