Proceedings of Materials for Sustainable Development Conference (MAT-SUS) (NFM22)
DOI: https://doi.org/10.29363/nanoge.nfm.2022.007
Publication date: 11th July 2022
Semiconductor polymeric carbon nitride (CNs) are a family of 2D materials that exhibit excellent photocatalytic properties for diverse chemical transformations thanks to their tunable band gap, suitable energy-band position, high stability under harsh chemical conditions, and low cost. Unfortunately, despite progress in the last decade, their utilization as the photoactive layer in photoelectrochemical (PEC) cells has yet to reach the performance of state-of-the-art metal-oxide-based systems. The main challenges thus far have been the difficulty in depositing high-quality and homogenous CN layers of controlled thickness on substrates, the wide band gap of ‘intrinsic’ CN ca. 2.7 eV, poor charge-separation efficiency, and low electronic conductivity.[1]
We present some noteworthy progress we have recently achieved in both stability and performance towards water-splitting as a result of tackling some of these limitations, mainly through variation of precursor deposition methods,[2–6] externally adding CN-precursor vapor during thermal polymerization,[5] incorporation of conductive carbons,[6,7] and successful incorporation of a NixFe1–xOyHz oxidation co-catalyst.[7] The latter is unique due to the difficulty of forming stable organic–inorganic heterojunctions in porous materials. This was accomplished by in-situ electrochemical transformation inside the porous CN matrix of a solvothermally-deposited pre-catalyst—a Ni/Fe-MIL-53 metal-organic framework (MOF)—into the co-catalyst. This configuration reaches photocurrents of 472 ± 20 µA cm–2 with faradaic efficiency towards O2 and H2 > 80% in 0.1 M KOH solution at 1.23 V vs. RHE. We show stable operation up to 35 h, where degradation occurs due to slow leaching of the co-catalyst.
This project received funding from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation programme (grant agreement no. [849068]) #MFreePEC.
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