Journal
CATALYSIS TODAY
Volume 287, Issue -, Pages 182-188Publisher
ELSEVIER
DOI: 10.1016/j.cattod.2016.11.007
Keywords
Photocatalysis; G-C-3 N-4; Synthesis temperature; Hydrogen production; Electron paramagnetic resonance
Funding
- SABIC
- EPSRC platform grant [EP/K015540/1]
- Royal Society of Chemistry for a Wolfson Merit Award
- EPSRC [EP/K015540/1] Funding Source: UKRI
- Engineering and Physical Sciences Research Council [EP/K015540/1] Funding Source: researchfish
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This work presents a systematic study of the effect of fabrication temperature (450 to 650 degrees C) on the structure and electronic properties of g-C-3 N-4 prepared from melamine. The work is conducted by X-ray diffraction, elemental analysis, BET nitrogen adsorption, UV-vis absorption, and electron paramagnetic resonance (EPR). The photocatalytic activity is tested for hydrogen production in the presence of oxalic acid (OA) as well as triethanolamine (TEOA). A considerable change in the morphology is observed with increasing the synthesis temperature resulting in an increase of the surface area, likely due to thermal etching. The decrease of charge carriers' concentration, per unit surface area, with increasing annealing temperature may be due to the decrease of the conjugation of the polymer. Probing the activity of in situ reduced Pt/g-C-3 N-4 for hydrogen evolution reinforced this conclusion, the rate of hydrogen evolution per unit area for OA as well as TEOA decreased with increasing annealing temperature. An interesting finding is the correlation between CO2:H-2 ratio and the increase in the band gap of g-C-3 N-4 prepared at different temperatures when using oxalic acid as an electron donor. This suggests that water oxidation becomes easier with increasing band gap energy, probably due to a lowering of the valence band edge. (C) 2016 Elsevier B.V. All rights reserved.
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