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Rational Design of Carbon Nitride Photoelectrodes with High Activity Toward Organic Oxidations.

Published version
Peer-reviewed

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Authors

Pulignani, Carolina 
Mesa, Camilo A 
Hillman, Sam AJ 
Uekert, Taylor 
Giménez, Sixto 

Abstract

Carbon nitride (CNx ) is a light-absorber with excellent performance in photocatalytic suspension systems, but the activity of CNx photoelectrodes has remained low. Here, cyanamide-functionalized CNx (NCN CNx ) was co-deposited with ITO nanoparticles on a 1.8 Å thick alumina-coated FTO electrode. Transient absorption spectroscopy and impedance measurements support that ITO acts as a conductive binder and improves electron extraction from the NCN CNx , whilst the alumina underlayer reduces recombination losses between the ITO and the FTO glass. The Al2 O3 |ITO : NCN CNx film displays a benchmark performance for CNx -based photoanodes with an onset of -0.4 V vs a reversible hydrogen electrode (RHE), and 1.4±0.2 mA cm-2 at 1.23 V vs RHE during AM1.5G irradiation for the selective oxidation of 4-methylbenzyl alcohol. This assembly strategy will improve the exploration of CNx in fundamental and applied photoelectrochemical (PEC) studies.

Description

Keywords

Carbon Nitride, Organic Oxidation, Photoanodes, Photoelectrochemistry, Spectroscopy

Journal Title

Angew Chem Int Ed Engl

Conference Name

Journal ISSN

1433-7851
1521-3773

Volume Title

Publisher

Wiley
Sponsorship
European Commission Horizon 2020 (H2020) Marie Sk?odowska-Curie actions (861151)
Engineering and Physical Sciences Research Council (EP/S022953/1)
Engineering and Physical Sciences Research Council (EP/L015978/1)
Engineering and Physical Sciences Research Council (EP/P030467/1)
Engineering and Physical Sciences Research Council (EP/P024947/1)
Engineering and Physical Sciences Research Council (EP/S019367/1)
Engineering and Physical Sciences Research Council (EP/R00661X/1)
EPSRC (via University of Manchester) (EP/X527257/1)