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Leaf-architectured 3D hierarchical artificial photosynthetic system of perovskite titanates towards CO? photoreduction into hydrocarbon fuels.

ABSTRACT: The development of an "artificial photosynthetic system" (APS) having both the analogous important structural elements and reaction features of photosynthesis to achieve solar-driven water splitting and CO? reduction is highly challenging. Here, we demonstrate a design strategy for a promising 3D APS architecture as an efficient mass flow/light harvesting network relying on the morphological replacement of a concept prototype-leaf's 3D architecture into perovskite titanates for CO? photoreduction into hydrocarbon fuels (CO and CH?). The process uses artificial sunlight as the energy source, water as an electron donor and CO? as the carbon source, mimicking what real leaves do. To our knowledge this is the first example utilizing biological systems as "architecture-directing agents" for APS towards CO? photoreduction, which hints at a more general principle for APS architectures with a great variety of optimized biological geometries. This research would have great significance for the potential realization of global carbon neutral cycle.

SUBMITTER: Zhou H

PROVIDER: S-EPMC3627189 | biostudies-literature | 2013

REPOSITORIES: biostudies-literature

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Leaf-architectured 3D hierarchical artificial photosynthetic system of perovskite titanates towards CO₂ photoreduction into hydrocarbon fuels.

Zhou Han H Guo Jianjun J Li Peng P Fan Tongxiang T Zhang Di D Ye Jinhua J

Scientific reports 20130101

The development of an "artificial photosynthetic system" (APS) having both the analogous important structural elements and reaction features of photosynthesis to achieve solar-driven water splitting and CO₂ reduction is highly challenging. Here, we demonstrate a design strategy for a promising 3D APS architecture as an efficient mass flow/light harvesting network relying on the morphological replacement of a concept prototype-leaf's 3D architecture into perovskite titanates for CO₂ photoreductio ...[more]

PMID: 23588925

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Project description:Photosynthetic reaction centers convert excitation energy from absorbed sunlight into chemical potential energy in the form of a charge-separated state. The rates of the electron transfer reactions necessary to achieve long-lived, high-energy charge-separated states with high quantum yields are determined in part by precise control of the electronic coupling among the chromophores, donors, and acceptors and of the reaction energetics. Successful artificial photosynthetic reaction centers for solar energy conversion have similar requirements. Control of electronic coupling in particular necessitates chemical linkages between active component moieties that both mediate coupling and restrict conformational mobility so that only spatial arrangements that promote favorable coupling are populated. Toward this end, we report the synthesis, structure, and photochemical properties of an artificial reaction center containing two porphyrin electron donor moieties and a fullerene electron acceptor in a macrocyclic arrangement involving a ring of 42 atoms. The two porphyrins are closely spaced, in an arrangement reminiscent of that of the special pair in bacterial reaction centers. The molecule is produced by an unusual cyclization reaction that yields mainly a product with C(2) symmetry and trans-2 disubstitution at the fullerene. The macrocycle maintains a rigid, highly constrained structure that was determined by UV-vis spectroscopy, NMR, mass spectrometry, and molecular modeling at the semiempirical PM6 and DFT (B3LYP/6-31G**) levels. Transient absorption results for the macrocycle in 2-methyltetrahydrofuran reveal photoinduced electron transfer from the porphyrin first excited singlet state to the fullerene to form a P(•+)-C(60)(•-)-P charge separated state with a time constant of 1.1 ps. Photoinduced electron transfer to the fullerene excited singlet state to form the same charge-separated state has a time constant of 15 ps. The charge-separated state is formed with a quantum yield of essentially unity and has a lifetime of 2.7 ns. The ultrafast charge separation coupled with charge recombination that is over 2000 times slower is consistent with a very rigid molecular structure having a small reorganization energy for electron transfer, relative to related porphyrin-fullerene molecules.

Dataset Information

Leaf-architectured 3D hierarchical artificial photosynthetic system of perovskite titanates towards CO? photoreduction into hydrocarbon fuels.

Publications

Leaf-architectured 3D hierarchical artificial photosynthetic system of perovskite titanates towards CO₂ photoreduction into hydrocarbon fuels.

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