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Cited by 420

The DOI matches its Crossref record; 30 of the 30 references it cites were found in a registry or an index.

Principles, Efficiency, and Blueprint Character of Solar-Energy Conversion in Photosynthetic Water Oxidation

Dau, Holger, Zaharieva, Ivelina·2009·Accounts of Chemical Research
DOI 10.1021/ar900225y
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Abstract

Photosynthesis in plants and cyanobacteria involves two protein-cofactor complexes which are denoted as photosystems (PS), PSII and PSI. These solar-energy converters have powered life on earth for approximately 3 billion years. They facilitate light-driven carbohydrate formation from H(2)O and CO(2), by oxidizing the former and reducing the latter. PSII splits water in a process driven by light. Because all attractive technologies for fuel production driven by solar energy involve water oxidation, recent interest in this process carried out by PSII has increased. In this Account, we describe and apply a rationale for estimating the solar-energy conversion efficiency (eta(SOLAR)) of PSII: the fraction of the incident solar energy absorbed by the antenna pigments and eventually stored in form of chemical products. For PSII at high concentrations, approximately 34% of the incident solar energy is used for creation of the photochemistry-driving excited state, P680*, with an excited-state energy of 1.83 eV. Subsequent electron transfer results in the reduction of a bound quinone (Q(A)) and oxidation of the Tyr(Z) within 1 micros. This radical-pair state is stable against recombination losses for approximately 1 ms. At this level, the maximal eta(SOLAR) is 23%. After the essentially irreversible steps of quinone reduction and water oxidation (the final steps catalyzed by the PSII complex), a maximum of 50% of the excited-state energy is stored in chemical form; eta(SOLAR) can be as high as 16%. Extending our considerations to a photosynthetic organism optimized to use PSII and PSI to drive H(2) production, the theoretical maximum of the solar-energy conversion efficiency would be as high as 10.5%, if all electrons and protons derived from water oxidation were used for H(2) formation. The above performance figures are impressive, but they represent theoretical maxima and do not account for processes in an intact organism that lower these yields, such as light saturation, photoinhibitory, protective, and repair processes. The overpotential for catalysis of water oxidation at the Mn(4)Ca complex of PSII may be as low as 0.3 V. To address the specific energetics of water oxidation at the Mn complex of PSII, we propose a new conceptual framework that will facilitate quantitative considerations on the basis of oxidation potentials and pK values. In conclusion, photosynthetic water oxidation works at high efficiency and thus can serve as both an inspiring model and a benchmark in the development of future technologies for production of solar fuels.

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Metadata

Authors
Dau, H., & Zaharieva, I.
Venue
Accounts of Chemical Research
Publisher
American Chemical Society (ACS)
Published
2009-11-12
Volume
42
Issue
12
Pages
1861-1870
ISSN
  • 0001-4842 (ISSN-L)
  • 1520-4898
DOI
10.1021/ar900225y
OpenAlex
W2163275303
Cited by
420
References
30
FWCI
9.48
Type
journal article
Language
en
Open access
closed

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