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At least 253 records · Page 14Linked to original sources
PubMed2006

All-solid-state Z-scheme in CdS-Au-TiO2 three-component nanojunction system.

Natural photosynthesis, which achieves efficient solar energy conversion through the combined actions of many types of molecules ingeniously arranged in a nanospace, highlights the importance of a technique for site-selective coupling of different materials to realize artificial high-efficiency devices. In view of increasingly serious energy and environmental problems, semiconductor-based artificial photosynthetic systems consisting of isolated photochemical system 1 (PS1), PS2 and the electron-transfer system have recently been developed. However, the direct coupling of the components is crucial for retarding back reactions to increase the reaction efficiency. Here, we report a simple technique for forming an anisotropic CdS-Au-TiO2 nanojunction, in which PS1(CdS), PS2(TiO2) and the electron-transfer system (Au) are spatially fixed. This three-component system exhibits a high photocatalytic activity, far exceeding those of the single- and two-component systems, as a result of vectorial electron transfer driven by the two-step excitation of TiO2 and CdS.

Journal Article↗
PubMed2005

Mechanisms of photoprotection and nonphotochemical quenching in pea light-harvesting complex at 2.5 A resolution.

The plant light-harvesting complex of photosystem II (LHC-II) collects and transmits solar energy for photosynthesis in chloroplast membranes and has essential roles in regulation of photosynthesis and in photoprotection. The 2.5 A structure of pea LHC-II determined by X-ray crystallography of stacked two-dimensional crystals shows how membranes interact to form chloroplast grana, and reveals the mutual arrangement of 42 chlorophylls a and b, 12 carotenoids and six lipids in the LHC-II trimer. Spectral assignment of individual chlorophylls indicates the flow of energy in the complex and the mechanism of photoprotection in two close chlorophyll a-lutein pairs. We propose a simple mechanism for the xanthophyll-related, slow component of nonphotochemical quenching in LHC-II, by which excess energy is transferred to a zeaxanthin replacing violaxanthin in its binding site, and dissipated as heat. Our structure shows the complex in a quenched state, which may be relevant for the rapid, pH-induced component of nonphotochemical quenching.

Binding Sites↗
PubMed2002

Fullerene-porphyrin architectures; photosynthetic antenna and reaction center models.

Fullerenes and porphyrins are molecular architectures ideally suited for devising integrated, multicomponent model systems to transmit and process solar energy. Implementation of C60 as a 3-dimensional electron acceptor holds great expectations on account of their small reorganization energy in electron transfer reactions and has exerted a noteworthy impact on the improvement of light-induced charge-separation. This article describes how the specific compositions of porphyrin chromophores linked to C60--yielding artificial light harvesting antenna and reaction center mimics--have been elegantly utilized to tune the electronic couplings between donor and acceptor sites and the total reorganization energy. Specifically, the effects that these parameters have on the rate, yield and lifetime of the energetic charge-separated states are considered.

Carbon↗
PubMed2004

Basic materials physics of transparent conducting oxides.

Materials displaying the remarkable combination of high electrical conductivity and optical transparency already from the basis of many important technological applications, including flat panel displays, solar energy capture and other opto-electronic devices. Here we present the basic materials physics of these important materials centred on the nature of the doping process to generate n-type conductivity in transparent conducting oxides, the associated transition to the metallic (conducting) state and the detailed properties of the degenerate itinerant electron gas. The aim is to fully understand the origins of the basic performance limits of known materials and to set the scene for new or improved materials which will breach those limits for new-generation transparent conducting materials, either oxides, or beyond oxides.

Journal Article↗
PubMed2005

Thermochemical solar hydrogen generation.

Solar direct, indirect and hybrid thermochemical processes are presented for the generation of hydrogen and compared to alternate solar hydrogen processes. A hybrid solar thermal/electrochemical process combines efficient photovoltaics and concentrated excess sub-bandgap heat into highly efficient elevated temperature solar electrolysis of water and generation of H2 fuel utilizing the thermodynamic temperature induced decrease of E(H2O) with increasing temperature. Theory and experiment is presented for this process using semiconductor bandgap restrictions and combining photodriven charge transfer, with excess sub-bandgap insolation to lower the water potential, and their combination into highly efficient solar generation of H2 is attainable. Fundamental water thermodynamics and solar photosensitizer constraints determine solar energy to hydrogen fuel conversion efficiencies in the 50% range over a wide range of insolation, temperature, pressure and photosensitizer bandgap conditions.

Journal Article↗
PubMed2004

Biophysical constraints on the origin of leaves inferred from the fossil record.

The molecular tool kit for producing flat-bladed photosynthetic structures evolved in marine and terrestrial plants during the middle Paleozoic, but it took a further 20 million years before leaves suddenly spread throughout land floras. This delay has long been difficult to explain, given the apparent advantage of leaves for photosynthetic primary production. Theory and experiments predict that exceptionally high atmospheric CO2 levels in the middle Paleozoic delayed the origin of leaves by restricting stomatal development. This would have limited evaporative cooling, leading to lethal overheating of leaves absorbing large quantities of solar energy. Here we test the central prediction of this argument with a morphometric analysis of 300 plant fossils from major European collections. We show a 25-fold enlargement of leaf blades in two phylogenetically independent clades as atmospheric CO2 levels fell during the late Paleozoic. Furthermore, preliminary data suggest that the first abrupt increase in leaf size was accompanied by an 8-fold rise in stomatal density. These evolutionary patterns support the relaxation of biophysical constraints on leaf area predicted by theory and point to a significant role for CO2 in plant evolution.

Atmosphere↗
PubMed2004

The long-range organization of a native photosynthetic membrane.

Photosynthesis relies on the delicate interplay between a specific set of membrane-bound pigment-protein complexes that harvest and transport solar energy, execute charge separation, and conserve the energy. We have investigated the organization of the light-harvesting (LH) and reaction-center (RC) complexes in native bacterial photosynthetic membranes of the purple bacterium Rhodobacter sphaeroides by using polarized light spectroscopy, linear dichroism (LD) on oriented membranes. These LD measurements show that in native membranes, which contain LH2 as the major energy absorber, the RC-LH1-PufX complexes are highly organized in a way similar to that which we found previously for a mutant lacking LH2. The relative contribution of LH1 and LH2 light-harvesting complexes to the LD spectrum shows that LH2 preferentially resides in highly curved parts of the membrane. Combining the spectroscopic data with our recent atomic force microscopy (AFM) results, we propose an organization for this photosynthetic membrane that features domains containing linear arrays of RC-LH1-PufX complexes interspersed with LH2 complexes and some LH2 found in separate domains. The study described here allows the simultaneous assessment of both global and local structural information on the organization of intact, untreated membranes.

Bacterial Proteins↗
PubMed2003

Early light-induced proteins protect Arabidopsis from photooxidative stress.

The early light-induced proteins (ELIPs) belong to the multigenic family of light-harvesting complexes, which bind chlorophyll and absorb solar energy in green plants. ELIPs accumulate transiently in plants exposed to high light intensities. By using an Arabidopsis thaliana mutant (chaos) affected in the posttranslational targeting of light-harvesting complex-type proteins to the thylakoids, we succeeded in suppressing the rapid accumulation of ELIPs during high-light stress, resulting in leaf bleaching and extensive photooxidative damage. Constitutive expression of ELIP genes in chaos before light stress resulted in ELIP accumulation and restored the phototolerance of the plants to the wild-type level. Free chlorophyll, a generator of singlet oxygen in the light, was detected by chlorophyll fluorescence lifetime measurements in chaos leaves before the symptoms of oxidative stress appeared. Our findings indicate that ELIPs fulfill a photoprotective function that could involve either the binding of chlorophylls released during turnover of pigment-binding proteins or the stabilization of the proper assembly of those proteins during high-light stress.

Arabidopsis↗
PubMed2000

The long-range supraorganization of the bacterial photosynthetic unit: A key role for PufX.

Bacterial photosynthesis relies on the interplay between light harvesting and electron transfer complexes, all of which are located within the intracytoplasmic membrane. These complexes capture and transfer solar energy, which is used to generate a proton gradient. In this study, we identify one of the factors that determines the organization of these complexes. We undertook a comparison of the organization of the light-harvesting complex 1 (LH1)/reaction center (RC) cores in the LH2(-) mutant of Rhodobacter sphaeroides in the presence or absence of the PufX protein. From polarized absorption spectra on oriented membranes, we conclude that PufX induces a specific orientation of the reaction center in the LH1 ring, as well as the formation of a long-range regular array of LH1-RC cores in the photosynthetic membrane. From our data, we have constructed a precise model of how the RC is positioned within the LH1 ring relative to the long (orientation) axis of the photosynthetic membrane.

Bacterial Proteins↗
PubMed2001

Indium-cadmium-oxide films having exceptional electrical conductivity and optical transparency: clues for optimizing transparent conductors.

Materials with high electrical conductivity and optical transparency are needed for future flat panel display, solar energy, and other opto-electronic technologies. In(x)Cd(1-x)O films having a simple cubic microstructure have been grown on amorphous glass substrates by a straightforward chemical vapor deposition process. The x = 0.05 film conductivity of 17,000 S/cm, carrier mobility of 70 cm2/Vs, and visible region optical transparency window considerably exceed the corresponding parameters for commercial indium-tin oxide. Ab initio electronic structure calculations reveal small conduction electron effective masses, a dramatic shift of the CdO band gap with doping, and a conduction band hybridization gap caused by extensive Cd 5s + In 5s mixing.

Journal Article↗
PubMed2001

Excited-state dynamics in photosystem II: insights from the x-ray crystal structure.

The heart of oxygenic photosynthesis is photosystem II (PSII), a multisubunit protein complex that uses solar energy to drive the splitting of water and production of molecular oxygen. The effectiveness of the photochemical reaction center of PSII depends on the efficient transfer of excitation energy from the surrounding antenna chlorophylls. A kinetic model for PSII, based on the x-ray crystal structure coordinates of 37 antenna and reaction center pigment molecules, allows us to map the major energy transfer routes from the antenna chlorophylls to the reaction center chromophores. The model shows that energy transfer to the reaction center is slow compared with the rate of primary electron transport and depends on a few bridging chlorophyll molecules. This unexpected energetic isolation of the reaction center in PSII is similar to that found in the bacterial photosystem, conflicts with the established view of the photophysics of PSII, and may be a functional requirement for primary photochemistry in photosynthesis. In addition, the model predicts a value for the intrinsic photochemical rate constant that is 4 times that found in bacterial reaction centers.

Crystallography, X-Ray↗
PubMed1973

Hydrogen evolution by a chloroplast-ferredoxin-hydrogenase system.

Spinach chloroplast preparations were mixed with Clostridium kluyveri hydrogenase and ferredoxin. Hydrogen evolution could be measured in the light in the absence of any added electron donors. Inhibition of the water-splitting reaction or of photosystem II reduced the amount of H(2) evolved more than 95%, indicating that H(2)O was the electron donor in this reaction. The rates of H(2) evolution observed were up to 20% of those measured in the presence of an oxygen-consuming reaction or of photosystem I electron donors. These findings indicate that hydrogen evolution from water and sunlight by photosynthetic processes could be a method for solar energy conversion.

Journal Article↗
PubMed1982

Photochemical generation of carbon monoxide and hydrogen by reduction of carbon dioxide and water under visible light irradiation.

Visible light irradiation of solutions of Ru(2,2'-bipyridine)(3) (2+), cobalt(II) chloride, and carbon dioxide in acetonitrile/water/triethylamine generates simultaneously carbon monoxide and hydrogen. The reaction involves photoinduced reduction of CO(2) and H(2)O, triethylamine serving as electron donor in the Ru(2,2'-bipyridine)(3) (2+)/Co(2+) system. The amount of gas (CO + H(2)) produced and the selectivity ratio CO/H(2) depend markedly on the composition of the system. Addition of free bipyridine strongly decreases CO generation but increases H(2) production. With different tertiary amines, NR(3), both the quantity (CO + H(2)) and the ratio CO/H(2) increase markedly along the sequence R = methyl, ethyl, propyl. Higher selectivity for CO(2) reduction to CO in preference to water reduction occurs when triethanolamine is used instead of triethylamine. CoCl(2) is the most efficient mediator for both CO and H(2) generation and specifically promotes CO formation, whereas salts of other cations studied only yield H(2). The mechanism of the reaction may involve intermediate formation of Co(I) species. These processes represent an abiotic photosynthetic system allowing simultaneous generation of CO and H(2) and regulation of the CO/H(2) ratio. Mechanistic studies and explorations of other components that may increase efficiency and product selectivity should be carried out. The results obtained are also of significance for solar energy conversion with consumption of a pollutant, CO(2).

Journal Article↗
PubMed1997

Efficient exchange of the primary quinone acceptor Q(A) in isolated reaction centers of Rhodopseudomonas viridis.

A key step in the conversion of solar energy into chemical energy by photosynthetic reaction centers (RCs) occurs at the level of the two quinones, Q(A) and Q(B), where electron transfer couples to proton transfer. A great deal of our understanding of the mechanisms of these coupled reactions relies on the seminal work of Okamura et al. [Okamura, M. Y., Isaacson, R. A., & Feher, G. (1975) Proc. Natl. Acad. Sci. USA 88, 3491-3495], who were able to extract with detergents the firmly bound ubiquinone Q(A) from the RC of Rhodobacter sphaeroides and reconstitute the site with extraneous quinones. Up to now a comparable protocol was lacking for the RC of Rhodopseudomonas viridis despite the fact that its Q(A) site, which contains 2-methyl-3-nonaprenyl-1,4-naphthoquinone (menaquinone-9), has provided the best x-ray structure available. Fourier transform infrared difference spectroscopy, together with the use of isotopically labeled quinones, can probe the interaction of Q(A) with the RC protein. We establish that a simple incubation procedure of isolated RCs of Rp. viridis with an excess of extraneous quinone allows the menaquinone-9 in the Q(A) site to be almost quantitatively replaced either by vitamin K(1), a close analogue of menaquinone-9, or by ubiquinone. To our knowledge, this is the first report of quinone exchange in bacterial photosynthesis. The Fourier transform infrared data on the quinone and semiquinone vibrations show a close similarity in the bonding interactions of vitamin K(1) with the protein at the Q(A) site of Rp. viridis and Rb. sphaeroides, whereas for ubiquinone these interactions are significantly different. The results are interpreted in terms of slightly inequivalent quinone-protein interactions by comparison with the crystallographic data available for the Q(A) site of the two RCs.

Journal Article↗
PubMed1998

Marine latitudinal diversity gradients: tests of causal hypotheses.

Latitudinal diversity gradients are first-order expressions of diversity patterns both on land and in the oceans, although the current hypotheses that seek to explain them are based chiefly on terrestrial data. We have assembled a database of the geographic ranges of 3,916 species of marine prosobranch gastropods living on the shelves of the western Atlantic and eastern Pacific Oceans, from the tropics to the Arctic Ocean. Western Atlantic and eastern Pacific diversities are similar, and the diversity gradients are strikingly similar despite many important physical and historical differences between the oceans. This shared diversity pattern cannot be explained by: (i) latitudinal differences in species range-length (Rapoport's rule); (ii) species-area effects; or (iii) recent geologic histories. One parameter that does correlate significantly with diversity in both oceans is solar energy input, as represented by average sea surface temperature. If this correlation is causal, sea surface temperature is probably linked to diversity through some aspect of productivity. In this case, diversity is an evolutionary outcome of trophodynamic processes inherent in ecosystems, and not just a byproduct of physical geographies.

Animals↗
PubMed1999

Biotechnology: enhancing human nutrition in developing and developed worlds.

While the last 50 years of agriculture have focused on meeting the food, feed, and fiber needs of humans, the challenges for the next 50 years go far beyond simply addressing the needs of an ever-growing global population. In addition to producing more food, agriculture will have to deal with declining resources like water and arable land, need to enhance nutrient density of crops, and achieve these and other goals in a way that does not degrade the environment. Biotechnology and other emerging life sciences technologies offer valuable tools to help meet these multidimensional challenges. This paper explores the possibilities afforded through biotechnology in providing improved agronomic "input" traits, differentiated crops that impart more desirable "output" traits, and using plants as green factories to fortify foods with valuable nutrients naturally rather than externally during food processing. The concept of leveraging agriculture as green factories is expected to have tremendous positive implications for harnessing solar energy to meet fiber and fuel needs as well. Widespread adaptation of biotech-derived products of agriculture should lay the foundation for transformation of our society from a production-driven system to a quality and utility-enhanced system.

Agriculture↗