TY  - GEN
A1  - Thiel, Kerstin
A1  - Zehbe, Rolf
A1  - Roeser, Jerômé
A1  - Strauch, Peter
A1  - Enthaler, Stephan
A1  - Thomas, Arne
T1  - A polymer analogous reaction for the formation of imidazolium and NHC based porous polymer networks
N2  - A polymer analogous reaction was carried out to generate a porous polymeric network with N-heterocyclic carbenes (NHC) in the polymer backbone. Using a stepwise approach, first a polyimine network is formed by polymerization of the tetrafunctional amine tetrakis(4-aminophenyl)methane. This polyimine network is converted in the second step into polyimidazolium chloride and finally to a polyNHC network. Furthermore a porous Cu(II)-coordinated polyNHC network can be generated. Supercritical drying generates polymer networks with high permanent surface areas and porosities which can be applied for different catalytic reactions. The catalytic properties were demonstrated for example in the activation of CO2 or in the deoxygenation of sulfoxides to the corresponding sulfides.
T3  - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 243 
KW  - covalent organic framework
KW  - n-heterocyclic carbenes
KW  - carbon-dioxide
KW  - intrinsic microporosity
KW  - heterogeneous catalysis
KW  - sulfoxides
KW  - reduction
KW  - complex
KW  - system
KW  - transformation
Y1  - 2013
U6  - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-95118
SP  - 1848
EP  - 1856
ER  - 
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
BT  - a combined first principles and semiempirical study
JF  - physical chemistry, chemical physics : PCCP
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 H₂ production O₂ evolution is only possible in the presence of oxidation cocatalysts.
KW  - initio molecular-dynamics
KW  - augmented-wave method
KW  - visible-light
KW  - tight-binding
KW  - transition
KW  - oxidation
KW  - photooxidation
KW  - simulations
KW  - reduction
KW  - hydrogen
Y1  - 2014
U6  - https://doi.org/10.1039/c4cp02021a
SN  - 1463-9076
SN  - 1463-9084
VL  - 2014
IS  - 16
SP  - 15917
EP  - 15926
ER  - 
TY  - GEN
A1  - Wirth, Jonas
A1  - Neumann, Rainer
A1  - Antonietti, Markus
A1  - Saalfrank, Peter
T1  - Adsorption and photocatalytic splitting of water on graphitic carbon nitride
BT  - a combined first principles and semiempirical study
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 H₂ production O₂ evolution is only possible in the presence of oxidation cocatalysts.
T3  - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - paper 172 
KW  - augmented-wave method
KW  - hydrogen
KW  - initio molecular-dynamics
KW  - oxidation
KW  - photooxidation
KW  - reduction
KW  - simulations
KW  - tight-binding
KW  - transition
KW  - visible-light
Y1  - 2014
U6  - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-74391
SP  - 15917
EP  - 15926
ER  -