Rational Design of Carbon Nitride Photoelectrodes with High Activity Toward Organic Oxidations
Carolina Pulignani, Camilo A. Mesa, Sam A. J. Hillman, Taylor Uekert, Sixto Giménez, James R. Durrant, Erwin Reisner
Abstract
Abstract Carbon nitride (CN x ) is a light‐absorber with excellent performance in photocatalytic suspension systems, but the activity of CN x photoelectrodes has remained low. Here, cyanamide‐functionalized CN x ( NCN CN x ) 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 CN x , whilst the alumina underlayer reduces recombination losses between the ITO and the FTO glass. The Al 2 O 3 |ITO : NCN CN x film displays a benchmark performance for CN x ‐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 CN x in fundamental and applied photoelectrochemical (PEC) studies.