TY  - JOUR
A1  - Wirth, Jonas
A1  - Neumann, Rainer
A1  - Antonietti, Markus
A1  - Saalfrank, Peter
T1  - Adsorption and photocatalytic splitting of water on graphitic carbon nitride: a combined first principles and semiempirical study
T2  - Physical chemistry, chemical physics : a journal of European Chemical Societies
N2  - Graphitic carbon nitride, g-C3N4, is a promising organic photo-catalyst for a variety of redox reactions. In order to improve its efficiency in a systematic manner, however, a fundamental understanding of the microscopic interaction between catalyst, reactants and products is crucial. Here we present a systematic study of water adsorption on g-C3N4 by means of density functional theory and the density functional based tight-binding method as a prerequisite for understanding photocatalytic water splitting. We then analyze this prototypical redox reaction on the basis of a thermodynamic model providing an estimate of the overpotential for both water oxidation and H+ reduction. While the latter is found to occur readily upon irradiation with visible light, we derive a prohibitive overpotential of 1.56 eV for the water oxidation half reaction, comparing well with the experimental finding that in contrast to H-2 production O-2 evolution is only possible in the presence of oxidation cocatalysts.
Y1  - 2014
UR  - https://publishup.uni-potsdam.de/frontdoor/index/index/docId/38258
SN  - 1463-9076
SN  - 1463-9084
VL  - 16
IS  - 30
SP  - 15917
EP  - 15926
PB  - Royal Society of Chemistry
CY  - Cambridge
ER  -