TY - JOUR
T1 - Light -induced charge separation across bio -inorganic interface
AU - Dimitrijevic, Nada M.
AU - De La Garza, Linda
AU - Rajh, Tijana
N1 - Funding Information:
The work was performed under the auspices of the U.S. Department of Energy, Office of Basic Energy Sciences under Contract No. DE-AC02-06CH11357.
PY - 2009/2/10
Y1 - 2009/2/10
N2 - Rational design of hybrid biomolecule nanoparticulate semiconductor conjugates enables coupling of functionality of biomolecules with the capability of semiconductors for solar energy capture, that can have potential application in energy conversion, sensing and catalysis. The particular challenge is to obtain efficient charge separation analogous to the natural photosynthesis process. The synthesis of axially anisotropic TiO2 nano-objects such as tubes, rods and bricks, as well as spherical and faceted nanoparticles has been developed in our laboratory. Depending on their size and shape, these nanostructures exhibit different domains of crystallinity, surface areas and aspect ratios. Moreover, in order to accommodate for high curvature in nanoscale regime, the surfaces of TiO2 nano-objects reconstructs resulting in changes in the coordination of surface Ti atoms from octahedral (D2d) to square pyramidal structures (C4v). The formation of these coordinatively unsaturated Ti atoms, thus depends strongly on the size and shape of nanocrystallites and affects trapping and reactivity of photogenerated charges. We have exploited these coordinatively unsaturated Ti atoms to coupe electron-donating (such as dopamine) and electron-accepting (pyrroloquinoline quinone) conductive linkers that allow wiring of biomolecules and proteins resulting in enhanced charge separation which increases the yield of ensuing chemical transformations.
AB - Rational design of hybrid biomolecule nanoparticulate semiconductor conjugates enables coupling of functionality of biomolecules with the capability of semiconductors for solar energy capture, that can have potential application in energy conversion, sensing and catalysis. The particular challenge is to obtain efficient charge separation analogous to the natural photosynthesis process. The synthesis of axially anisotropic TiO2 nano-objects such as tubes, rods and bricks, as well as spherical and faceted nanoparticles has been developed in our laboratory. Depending on their size and shape, these nanostructures exhibit different domains of crystallinity, surface areas and aspect ratios. Moreover, in order to accommodate for high curvature in nanoscale regime, the surfaces of TiO2 nano-objects reconstructs resulting in changes in the coordination of surface Ti atoms from octahedral (D2d) to square pyramidal structures (C4v). The formation of these coordinatively unsaturated Ti atoms, thus depends strongly on the size and shape of nanocrystallites and affects trapping and reactivity of photogenerated charges. We have exploited these coordinatively unsaturated Ti atoms to coupe electron-donating (such as dopamine) and electron-accepting (pyrroloquinoline quinone) conductive linkers that allow wiring of biomolecules and proteins resulting in enhanced charge separation which increases the yield of ensuing chemical transformations.
KW - Charge transfer complex
KW - Extended charge separation
KW - Phonon interactions
KW - Titanium dioxide
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U2 - 10.1142/S0217979209049942
DO - 10.1142/S0217979209049942
M3 - Article
AN - SCOPUS:67849097410
SN - 0217-9792
VL - 23
SP - 473
EP - 491
JO - International Journal of Modern Physics B
JF - International Journal of Modern Physics B
IS - 4
ER -