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What Nanoporous Supports Do We Need for Solar Light-Driven Fuel Synthesis . Direct Solar to Fuel by Solid Photocatalysts Principle:. Direct Solar to Fuel by Solid Photocatalysts. Where we are: UV light-driven Water Splitting: mixed metal oxide nanoparticles.
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Direct Solar to Fuel by Solid Photocatalysts
Where we are:
UV light-driven Water Splitting: mixed metal oxide nanoparticles
Kudo, J. Am. Chem. Soc.2003, 125, 3082.
Q.Y. = 56%, > 400 hours
● Direct solar to fuel works with UV light
Where we are: UV light-driven CO2 reduction by H2O: Isolated Ti
centers in nanoporous silicate
● Direct Solar to Fuel Works with UV Light
Anpo, Catal. Today1998, 44, 327
Frei, J. Phys. Chem. B2004, 108, 18269
Single Component mixed metal oxide
Two-component mixed metal oxide
with shuttle (Z-scheme)
Q.Y.= 0.3% at 420 nm
Arakawa, Science2001, 414, 625
Q.Y.= 0.3% at 500 nm
Kudo, Chem. Commun. 2001, 2416
Where we are: Visible light-driven CO2 Splitting
Binuclear photocatalytic sites on inert mesoporous oxide support
Frei, J. Am. Chem. Soc. 2005, 127, 1610
Numerous small bandgap semiconductor photocatalysts work efficiently under visible light (λ>600 nm, q.y.>50%), but require sacrificial reagents
Lesson: no defects or ill-defined structures can be involved in energy transduction, charge migration, or catalytic transformation because they will invariably lead to loss of stored energy, charge, or chemical selectivity
How can we avoid sacrificial reagents:
exploit gas-solid interface
Ru(bpy)32+ sensitizer/ Ni(cyclam) catalyst (CO2 to CO, H2O reduction)
IrOx Clusters (H2O oxidation)
MMCT units (CO2 splitting)
Challenge: Incorporation of organic and polynuclear transition metal units at preselected sites and defined orientation inside silica wall
Challenge: Ir oxide patches of defined composition and structure covalently linked to Co-O-Ti units inside mesoporous silica wall
Develop methods that afford imprinting of molecular components and well-defined metal oxide clusters into walls of mesoporous nonreducible oxide supports at predetermined locations and with defined orientation
New types of templates
Methods for creating channel patterns with oxidizing/reducing sites
Defect-free active component/silica interface
Design new catalytic components for coupled H2O oxidation/CO2 reduction