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Potassium Poly(heptazine imides) from Aminotetrazoles: Shifting Band Gaps of Carbon Nitride-like Materials for More Efficient Solar Hydrogen and Oxygen Evolution

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http://pubman.mpdl.mpg.de/cone/persons/resource/persons22243

Willinger,  Marc Georg
Department of Colloid Chemistry Max-Planck Institute of Colloids and Interfaces;
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Citation

Savateev, A., Pronkin, S., Epping, J. D., Willinger, M. G., Wolff, C., Neher, D., et al. (2017). Potassium Poly(heptazine imides) from Aminotetrazoles: Shifting Band Gaps of Carbon Nitride-like Materials for More Efficient Solar Hydrogen and Oxygen Evolution. ChemCatChem, 9(1), 167-174. doi:10.1002/cctc.201601165.


Cite as: http://hdl.handle.net/11858/00-001M-0000-002C-5583-8
Abstract
Potassium poly(heptazine imide) (PHI) is a photocatalytically active carbon nitride material that was recently prepared from substituted 1,2,4-triazoles. Here, we show that the more acidic precursors, such as commercially available 5-aminotetrazole, upon pyrolysis in LiCl/KCl salt melt yield PHI with the greatly improved structural order and thermodynamic stability. Tetrazole-derived PHIs feature long-range crystallinities and unconventionally small layer stacking distances, leading to the altered electronic band structures as shown by Mott–Schottky analyses. Under the optimized synthesis conditions, visible-light driven hydrogen evolution rates reach twice the rate provided by the previous gold standard, mesoporous graphitic carbon nitride, which has a much higher surface area. More interestingly, the up to 0.7 V higher valence band potential of crystalline PHI compared with ordinary carbon nitrides makes it an efficient water oxidation photocatalyst, which works even in the absence of any metal-based co-catalysts under visible light. To our knowledge, this is the first case of metal-free oxygen liberation from water.