Publication date: 21st July 2025
Two-dimensional materials in the carbon nitride family have recently garnered attention for their ability
to function as photocatalysts under visible light. However, their application as thin films have been
limited due to poor coating homogeneity. We have developed an innovative chemical vapor deposition
(CVD) method that enables the deposition of carbon nitride thin films with tuneable thickness and high
uniformity.1 The conformal nature of these CVD-grown films allows integration into microfluidic
reactors, where they demonstrate superior performance in the photocatalytic oxidation of benzylic
alcohols under flow conditions.2 Furthermore, the homogeneity of the films facilitates the use of
advanced spectroscopic techniques—including NMR, XPS, and XAS—for in-operando analysis of
photocatalytic reaction mechanisms. Using in-operando XPS and XAS, we explored the mechanism of
photocatalytic water splitting, uncovering the crucial role of surface interactions, particularly the
formation of hydrogen bonds with water, in activating the carbon nitride surface. Upon illumination we
were able to confirm the evolution of hydrogen and oxygen while the spectroscopic features recorded
support the proton-coupled electron transfer (PCET) mechanism. These insights provide a fundamental
understanding of one of the most extensively studied reactions of the past decade, both experimentally
and theoretically. Although the use of thin films in energy conversion is still emerging, our work
highlights their potential to drive significant progress in photocatalysis, photoelectrocatalysis, and
beyond.
Keywords: carbon nitride, thin films, artificial photosynthesis, water splitting
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