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Abstract
A general synthesis of carbon nitride (CN) films with extended optical absorption, excellent charge separation under illumination, and outstanding performance as a photoanode in water-splitting photoelectrochemical cells is reported. To this end, we introduced a universal method to rapidly grow CN monomers directly from a hot saturated solution on various substrates. Upon calcination, a highly uniform carbon nitride layer with tuned structural and photophysical properties and in intimate contact with the substrate is obtained. Detailed photoelectrochemical and structural studies reveal good photoresponse up to 600 nm, excellent hole extraction efficiency (up to 62%) and strong adhesion of the CN layer to the substrate. The best CN photoanode demonstrates a benchmark-setting photocurrent density of 353 µA cm−2 (51% faradaic efficiency for oxygen), and external quantum yield value above 12% at 450 nm at 1.23 V versus RHE in an alkaline solution, as well as low onset potential and good stability.
Highlights
A general synthesis of carbon nitride (CN) films with extended optical absorption, excellent charge separation under illumination, and outstanding performance as a photoanode in water-splitting photoelectrochemical cells is reported
Taking urea as an example, we showed that a uniform and ordered urea film on fluorine-doped tin oxide (FTO) can be obtained by using this method (Supplementary Fig. 14)
The reported simple, scalable, and versatile method allows the deposition of uniform carbon nitride layers with enhanced optical absorption and charge separation under illumination on various substrates
Summary
A general synthesis of carbon nitride (CN) films with extended optical absorption, excellent charge separation under illumination, and outstanding performance as a photoanode in water-splitting photoelectrochemical cells is reported. To this end, we introduced a universal method to rapidly grow CN monomers directly from a hot saturated solution on various substrates. We demonstrate a simple and general method to grow porous CN films with extended optical absorption, improved charge separation properties under illumination, and intimate contact with the substrate via the direct and fast growth of monomers from saturated solutions, followed by calcination at high temperature. Gas evolution rates of 1.88 μmol h−1 cm−2 for H2 and 0.91 μmol h−1 cm−2 for O2 are detected
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