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@ARTICLE{Koposova:811872,
author = {Koposova, Ekaterina and Liu, Xiao and Pendin, Andrey and
Thiele, Björn and Shumilova, Galina and Ermolenko, Yury and
Offenhäusser, Andreas and Mourzina, Youlia},
title = {{I}nfluence of {M}eso-{S}ubstitution of the {P}orphyrin
{R}ing on {E}nhanced {H}ydrogen {E}volution in a
{P}hotochemical {S}ystem},
journal = {The journal of physical chemistry / C},
volume = {120},
number = {26},
issn = {1932-7455},
address = {Washington, DC},
publisher = {Soc.},
reportid = {FZJ-2016-04214},
pages = {13873 - 13890},
year = {2016},
abstract = {This study establishes the relationships between the
structure of a series of meso-substituted tin(IV) porphyrins
and their efficiency as photosensitizers for hydrogen
generation in the Sn(IV)P/Pt–TiO2 nanocomposite system.
The electrochemical properties of a series of SnPs, the
catalytic performance of Pt nanomodifications, and the
morphology of the Pt/TiO2 nanocomposites were characterized
by electrochemical and electron microscopy methods. The
dependence of photocatalytic performance on the structure
for a series of Sn(IV) meso-substituted phenyl porphyrins
was studied, and possible mechanisms are discussed employing
the results of the electrochemical studies. It was found
that the time course and type of the photochemically reduced
species of Sn(IV)Ps, which are essential intermediates, are
important factors and depend on the electronegativity of the
metal center, the character of meso-substituents of the
porphyrin ring, and pH and are correlated with the redox
potential sequence of the respective Sn(IV)Ps: SnTMPyP >
SnTPyP > SnTPPS > SnTPPC. Optimization of the experimental
parameters was performed with regard to the SnPs with
different functional groups, pH values, concentrations of
Pt/TiO2, light intensity, and Pt nanoparticles with
different surface stabilizers. Finally, the maximum hydrogen
yield under visible light was obtained from the system of
Sn(IV) meso-tetra(4-pyridyl)porphyrin dichloride (SnTPyP)
sensitized TiO2/Pt prepared by the citrate method/EDTA at pH
9.0. This demonstrates that the photochemically reduced
species of SnTPyP are relatively long lived, so they have
enough time to complete electron transfer to TiO2 and/or Pt.
The adsorption of SnTPyP on the TiO2/Pt surface is therefore
not essential for hydrogen generation. Moreover, this study
demonstrates for the first time the synergic effect of the
excitation of TiO2 and mostly Q-bands of Sn(IV)P (wavelength
range 390–650 nm), which enhances the efficiency of
photocatalytic hydrogen generation in the system. The Soret
band of Sn(IV)TPyP was found to produce a minor (about
$23\%)$ contribution to the photocatalytic activity of the
porphyrin sensitizer in this system. Possible processes
involved are discussed, and mechanisms are proposed
explaining different aspects of a series of photocatalytic
systems with SnPs and Pt catalysts for hydrogen production
under visible light. These structure–function
relationships are essential to effectively harness solar
energy for hydrogen production as well as for a wide range
of energy and environmentally related problems.},
cin = {PGI-8 / IBG-2},
ddc = {540},
cid = {I:(DE-Juel1)PGI-8-20110106 / I:(DE-Juel1)IBG-2-20101118},
pnm = {134 - Electrolysis and Hydrogen (POF3-134) / 582 - Plant
Science (POF3-582)},
pid = {G:(DE-HGF)POF3-134 / G:(DE-HGF)POF3-582},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000379457000003},
doi = {10.1021/acs.jpcc.6b01467},
url = {https://juser.fz-juelich.de/record/811872},
}