@article{WirthNeumannAntoniettietal.2014,
  author    = {Wirth, Jonas and Neumann, Rainer and Antonietti, Markus and Saalfrank, Peter},
  title     = {Adsorption and photocatalytic splitting of water on graphitic carbon nitride},
  series = {physical chemistry, chemical physics : PCCP},
  volume    = {2014},
  journal   = {physical chemistry, chemical physics : PCCP},
  number    = {16},
  issn      = {1463-9076},
  doi       = {10.1039/c4cp02021a},
  pages     = {15917 -- 15926},
  year      = {2014},
  abstract  = {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.},
  language  = {en}
}
@article{ZamponiPenfoldNachtegaaletal.2014,
  author    = {Zamponi, Flavio and Penfold, Thomas J. and Nachtegaal, Maarten and L{\"u}bcke, Andrea and Rittmann, Jochen and Milne, Chris J. and Chergui, Majed and van Bokhoven, Jeroen A.},
  title     = {Probing the dynamics of plasmon-excited hexanethiol-capped gold nanoparticles by picosecond X-ray absorption spectroscopy},
  series = {physical chemistry, chemical physics : PCCP},
  volume    = {2014},
  journal   = {physical chemistry, chemical physics : PCCP},
  number    = {16},
  issn      = {1463-9076},
  doi       = {10.1039/c4cp03301a},
  pages     = {23157 -- 23163},
  year      = {2014},
  abstract  = {Picosecond X-ray absorption spectroscopy (XAS) is used to investigate the electronic and structural dynamics initiated by plasmon excitation of 1.8 nm diameter Au nanoparticles (NPs) functionalised with 1-hexanethiol. We show that 100 ps after photoexcitation the transient XAS spectrum is consistent with an 8\% expansion of the Au-Au bond length and a large increase in disorder associated with melting of the NPs. Recovery of the ground state occurs with a time constant of ∼1.8 ns, arising from thermalisation with the environment. Simulations reveal that the transient spectrum exhibits no signature of charge separation at 100 ps and allows us to estimate an upper limit for the quantum yield (QY) of this process to be <0.1.},
  language  = {en}
}
@misc{ZamponiPenfoldNachtegaaletal.2014,
  author    = {Zamponi, Flavio and Penfold, Thomas J. and Nachtegaal, Maarten and L{\"u}bcke, Andrea and Rittmann, Jochen and Milne, Chris J. and Chergui, Majed and van Bokhoven, Jeroen A.},
  title     = {Probing the dynamics of plasmon-excited hexanethiol-capped gold nanoparticles by picosecond X-ray absorption spectroscopy},
  url       = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-74492},
  pages     = {23157 -- 23163},
  year      = {2014},
  abstract  = {Picosecond X-ray absorption spectroscopy (XAS) is used to investigate the electronic and structural dynamics initiated by plasmon excitation of 1.8 nm diameter Au nanoparticles (NPs) functionalised with 1-hexanethiol. We show that 100 ps after photoexcitation the transient XAS spectrum is consistent with an 8\% expansion of the Au-Au bond length and a large increase in disorder associated with melting of the NPs. Recovery of the ground state occurs with a time constant of ∼1.8 ns, arising from thermalisation with the environment. Simulations reveal that the transient spectrum exhibits no signature of charge separation at 100 ps and allows us to estimate an upper limit for the quantum yield (QY) of this process to be <0.1.},
  language  = {en}
}
@misc{WirthNeumannAntoniettietal.2014,
  author    = {Wirth, Jonas and Neumann, Rainer and Antonietti, Markus and Saalfrank, Peter},
  title     = {Adsorption and photocatalytic splitting of water on graphitic carbon nitride},
  url       = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-74391},
  pages     = {15917 -- 15926},
  year      = {2014},
  abstract  = {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.},
  language  = {en}
}