Proceedings of MATSUS Spring 2024 Conference (MATSUS24)
DOI: https://doi.org/10.29363/nanoge.matsus.2024.463
Publication date: 18th December 2023
Polymeric carbon nitride (CN) has emerged as a promising photoanode material in photoelectrochemical cells (PEC) thanks to its cost-effectiveness, lack of toxic or rare elements, high chemical stability, and suitable band edge positions (for common redox reactions as water-splitting and a band gap in visible range.1–3 However, CN faces several challenges as an active photoanodic material due to its inherent moderate light-harvesting capabilities and inadequate exciton separation properties. These intrinsic properties, combined with the difficulty in establishing intimate contact with the substrate, hinder the successful application of CN in PEC systems. Controlling the properties of a CN layer during its in–situ growth on a conductive substrate, including its directionality, morphology, surface area, and defects, is challenging because of the high temperature of the reaction and the substrate properties. Here, we report the growth of defect–rich, porous 1D CN with enhanced optical properties and photocatalytic activity by utilizing sophisticated supramolecular assemblies composed of melamine and HCl as starting precursors. The supramolecular assembly composition directs the 1D growth, and the presence of protonated amines in the precursor leads to partial condensation and defect generation. The 1D configuration, high surface area, and abundance of defects of the photoanode result in high photoelectrochemical activity for water and benzylamine oxidation. The new design of the CN photoanode leads to very low overpotential, good photocurrent density of 183 ± 8 μA cm−2 at 1.23 V vs. RHE, with an incident photon to current efficiency (IPCE) of up to 10.5% and enhanced stability (retaining ~62% activity) for 10 h. Moreover, the conversion of benzylamine into benzaldehyde and imine N–benzylideneaniline in the presence of O2 reaches 56% compared to 16% for the reference CN photoanode.
This project has received funding from the European Research Council (ERC) under the European Union's Horizon 2020 Research and Innovation Programme (Grant Agreement No. 849068). This work was partially supported by the Israel Science Foundation, Grant No. 601/21.
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