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Biomimetic and Microbial Approaches to Solar Fuel Generation

Magnuson, Ann; Anderlund, Magnus; Johansson, Olof; Lindblad, Peter; Lomoth, Reiner; Polivka, Tomas LU ; Ott, Sascha; Stensjo, Karin; Styring, Stenbjorn and Sundström, Villy LU , et al. (2009) In Accounts of Chemical Research 42(12). p.1899-1909
Abstract
Photosynthesis is performed by a multitude of organisms, but in P nearly all cases, it is variations on a common theme: absorption of light followed by energy transfer to a reaction center where charge separation takes place, This initial form of chemical energy is stabilized by the biosynthesis of carbohydrates. To produce these energy-rich products, a substrate is needed that feeds in reductive equivalents, When photosynthetic microorganisms learned to use water as a substrate some 2 billion years ago, a fundamental barrier against unlimited use of solar energy was overcome. The possibility of solar energy use has inspired researchers to construct artificial photosynthetic systems that show analogy to parts of the intricate molecular... (More)
Photosynthesis is performed by a multitude of organisms, but in P nearly all cases, it is variations on a common theme: absorption of light followed by energy transfer to a reaction center where charge separation takes place, This initial form of chemical energy is stabilized by the biosynthesis of carbohydrates. To produce these energy-rich products, a substrate is needed that feeds in reductive equivalents, When photosynthetic microorganisms learned to use water as a substrate some 2 billion years ago, a fundamental barrier against unlimited use of solar energy was overcome. The possibility of solar energy use has inspired researchers to construct artificial photosynthetic systems that show analogy to parts of the intricate molecular machinery of photosynthesis. Recent years have seen a reorientation of efforts toward creating integrated light-to-fuel systems that can use solar energy for direct synthesis of energy-rich compounds, so-called solar fuels. Sustainable production of solar fuels is a long awaited development that promises extensive solar energy use combined with long-term storage. The stoichiometry of water splitting into molecular oxygen, protons, and electrons is deceptively simple; achieving it by chemical catalysis has proven remarkably difficult. The reaction center Photosystem II couples light-induced charge separation to an efficient molecular water-splitting catalyst, a Mn4Ca complex, and is thus an important template for biomimetic chemistry. In our aims to design biomimetic manganese complexes for light-driven water oxidation, we link photosensitizers and charge-separation motifs to potential catalysts in supramolecular assemblies. In photosynthesis, production of carbohydrates demands the delivery of multiple reducing equivalents to CO2. In contrast, the two-electron reduction of protons to molecular hydrogen is much less demanding. Virtually all microorganisms have enzymes called hydrogenases that convert protons to hydrogen, many of them with good catalytic efficiency. The catalytic sites of hydrogenases are now the center of attention of biomimetic efforts, providing prospects for catalytic hydrogen production with inexpensive metals. Thus, we might complete the water-to-fuel conversion: light + 2H(2)O -> 2H(2) + O-2 This reaction formula is to some extent already elegantly fulfilled by cyanobacteria and green algae, water-splitting photosynthetic microorganisms that under certain conditions also can produce hydrogen. An alternative route to hydrogen from solar energy is therefore to engineer these organisms to produce hydrogen more efficiently. This Account describes our original approach to combine research in these two fields: mimicking structural and functional principles of both Photosystem II and hydrogenases by synthetic chemistry and engineering cyanobacteria to become better hydrogen producers and ultimately developing new routes toward synthetic biology. (Less)
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Accounts of Chemical Research
volume
42
issue
12
pages
1899 - 1909
publisher
The American Chemical Society
external identifiers
  • wos:000273082800006
  • scopus:72949084589
ISSN
1520-4898
DOI
10.1021/ar900127h
language
English
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yes
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58b7a2af-335f-4c6b-8dce-2fad426eb040 (old id 1531792)
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2010-01-28 16:53:55
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@article{58b7a2af-335f-4c6b-8dce-2fad426eb040,
  abstract     = {Photosynthesis is performed by a multitude of organisms, but in P nearly all cases, it is variations on a common theme: absorption of light followed by energy transfer to a reaction center where charge separation takes place, This initial form of chemical energy is stabilized by the biosynthesis of carbohydrates. To produce these energy-rich products, a substrate is needed that feeds in reductive equivalents, When photosynthetic microorganisms learned to use water as a substrate some 2 billion years ago, a fundamental barrier against unlimited use of solar energy was overcome. The possibility of solar energy use has inspired researchers to construct artificial photosynthetic systems that show analogy to parts of the intricate molecular machinery of photosynthesis. Recent years have seen a reorientation of efforts toward creating integrated light-to-fuel systems that can use solar energy for direct synthesis of energy-rich compounds, so-called solar fuels. Sustainable production of solar fuels is a long awaited development that promises extensive solar energy use combined with long-term storage. The stoichiometry of water splitting into molecular oxygen, protons, and electrons is deceptively simple; achieving it by chemical catalysis has proven remarkably difficult. The reaction center Photosystem II couples light-induced charge separation to an efficient molecular water-splitting catalyst, a Mn4Ca complex, and is thus an important template for biomimetic chemistry. In our aims to design biomimetic manganese complexes for light-driven water oxidation, we link photosensitizers and charge-separation motifs to potential catalysts in supramolecular assemblies. In photosynthesis, production of carbohydrates demands the delivery of multiple reducing equivalents to CO2. In contrast, the two-electron reduction of protons to molecular hydrogen is much less demanding. Virtually all microorganisms have enzymes called hydrogenases that convert protons to hydrogen, many of them with good catalytic efficiency. The catalytic sites of hydrogenases are now the center of attention of biomimetic efforts, providing prospects for catalytic hydrogen production with inexpensive metals. Thus, we might complete the water-to-fuel conversion: light + 2H(2)O -> 2H(2) + O-2 This reaction formula is to some extent already elegantly fulfilled by cyanobacteria and green algae, water-splitting photosynthetic microorganisms that under certain conditions also can produce hydrogen. An alternative route to hydrogen from solar energy is therefore to engineer these organisms to produce hydrogen more efficiently. This Account describes our original approach to combine research in these two fields: mimicking structural and functional principles of both Photosystem II and hydrogenases by synthetic chemistry and engineering cyanobacteria to become better hydrogen producers and ultimately developing new routes toward synthetic biology.},
  author       = {Magnuson, Ann and Anderlund, Magnus and Johansson, Olof and Lindblad, Peter and Lomoth, Reiner and Polivka, Tomas and Ott, Sascha and Stensjo, Karin and Styring, Stenbjorn and Sundström, Villy and Hammarstrom, Leif},
  issn         = {1520-4898},
  language     = {eng},
  number       = {12},
  pages        = {1899--1909},
  publisher    = {The American Chemical Society},
  series       = {Accounts of Chemical Research},
  title        = {Biomimetic and Microbial Approaches to Solar Fuel Generation},
  url          = {http://dx.doi.org/10.1021/ar900127h},
  volume       = {42},
  year         = {2009},
}