Thermodynamic analysis of energy conversion from light-to-chemical, light-to-electric and electric-to-chemical is presented by the case study of water photoelectrolysis on TiO₂ surface. It is demonstrated that at the current state-of-the-art energy conversion efficiency of water photoelectrolysis can be increased ∼17 times by separating the processes of solar-to-electric and electric-to-chemical energy conversion and optimizing them independently. This allows to mitigate a high overvoltage of oxygen evolution reaction with respect to thermodynamic $E_{O_2/H_{2}O}^0\hspace{0.17em}=1.23\hspace{0.17em}\text{V}$ potential as well as spectrally narrow absorbtivity of solar light by TiO₂ which determine the low efficiency (∼ 1.0%) of direct light-to-chemical energy conversion. Numerical estimates are provided illustrating practical principles for optimization of the solar energy conversion and storage processes.

© 2010 Optical Society of America

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49. J. Lee, J. Park, J. Kim, D. Lee, and K. Cho, "High efficiency polymer solar cells with wet deposited plasmonic gold nanodots," Org. Electron. 10, 416-420 (2009). [CrossRef]
50. Y. Tian and T. Tatsuma, "Mechanismsand applications of plasmon-induced charge separationat tio2 films loaded with gold nanoparticles," J. Am. Chem. Soc. 127, 7632-7637 (2005). [CrossRef] [PubMed]
51. C. Chou, R. Yang, C. Yeh, and Y. Lin, "Preparation of tio2/nano-metal composite particles and thier applications in dye-sensitized solar cells," Powder Technol. 194, 95-105 (2009). [CrossRef]
52. T. Hasobe, H. Imahori, S. Fukuzumi, and P. V. Kamat, "Nanostructured assembly of porphyrin clusters for light energyconversion," J. Mater. Chem. 13, 2515-2520 (2003). [CrossRef]
53. H. Imahori and T. Umeyama, "Donor-acceptor nanoarchitecture on semiconducting electrodes forsolar energy conversion," J. Phys. Chem. C 113, 9029-9039 (2009). [CrossRef]
54. Y. Yokota, K. Ueno, V. Mizeikis, S. Juodkazis, K. Sasaki, and H. Misawa, "Optical characterization of plasmonic metallic nanostructures fabricated by high-resolution lithography," J. Nanophoton. 1, 011594 (2008). [CrossRef]
55. K. Ueno, S. Juodkazis, V. Mizeikis, K. Sasaki, and H. Misawa, "Clusters of closely spaced gold nanoparticles as a source of two-photon photoluminescence at visible wavelengths," Adv. Mater. 20, 26 - 29 (2008). [CrossRef]
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57. K. Ueno, S. Juodkazis, V. Mizeikis, K. Sasaki, and H. Misawa, "Spectrally-resolved atomic-scale variations of gold nanorods," J. Am. Chem. Soc. 128, 14226-14227 (2006). [CrossRef] [PubMed]
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62. L. Carrette, K.A. Friedrich, and U. Stimming, "Fuel cells: Fundamentals and applications," Fuel Cells 1, 5-39 (2001). [CrossRef]

Acc. Chem. Res.

• B. Parkinson, "On the efficiency and stability of photoelectrochemical. devices," Acc. Chem. Res. 17, 431 - 437 (1984). [CrossRef]

Adv. Mater.

• E. Hutter and J. H. Fendler, "Exploitation of localized surface plasmon resonance," Adv. Mater. 16, 1686- 1708 (2004). [CrossRef]
• K. Ueno, S. Juodkazis, V. Mizeikis, K. Sasaki, and H. Misawa, "Clusters of closely spaced gold nanoparticles as a source of two-photon photoluminescence at visible wavelengths," Adv. Mater. 20, 26 - 29 (2008). [CrossRef]

Appl. Phys. Lett.

• K. A. Bertness, S. R. Kurtz, D. J. Friedman, and A. E. Kibbler, "29.5 percent-efficient GaInP/GaAs tandem solar cells," Appl. Phys. Lett. 65, 989-991 (1994). [CrossRef]
• J. H. Zhao, A. H. Wang, M. A. Green, and F. Ferrazza, "19.8% efficient "honeycomb" textured multicrystalline and 24.4% monocrystalline silicon solar cells," Appl. Phys. Lett. 73, 1991-1993 (1998). [CrossRef]

Chem. Rev.

• A. L. Linsebigler, G. Lu, and J.T. Yates, "Photocatalysis on TiO2 surfaces: Principles, mechanisms, and selected results," Chem. Rev. 95, 735 - 758 (1995). [CrossRef]

Chemija

• A. Survila, P. Kalinauskas, and I. Valsi?nas, "Photoelektrochemical properties of surface layers formed by anodic oxidation of titanium," Chemija 10, 117 - 121 (1999).
• K. Juodkazis, J. Juodkazyt?, R. Vilkauskait?, B. Šebeka, and V. Jasulaitien?, "Oxygen evolution on mixed ruthenium and nickel oxide electrode," Chemija 19, 1 - 6 (2008).

Electrochem. Commun.

• R. Beranek and H. Kisch, "Surface-modified anodic TiO2 films for visible light photocurrent response," Electrochem. Commun. 9, 761-766 (2007). [CrossRef]
• T. Lana-Villarreal and R. Gomez, "Interfacial electron transfer at TiO2 nanostructured electrodes modified with capped gold nanoparticles: The photoelectrochemistry of water oxidation," Electrochem. Commun. 7, 1218-1224 (2005). [CrossRef]

Electrochimica Acta

• K. Juodkazis, J. Juodkazyt?, T. Juodien?, V. Šukien?, and I. Savickaja, "Alternative view of anodic surface oxidation of noble metals," Electrochimica Acta 51, 6159 - 6164 (2006). [CrossRef]

Fuel Cells

• L. Carrette, K.A. Friedrich, and U. Stimming, "Fuel cells: Fundamentals and applications," Fuel Cells 1, 5-39 (2001). [CrossRef]

Int. J. Hydr. Energ.

• J. Nowotny, T. Bak, M. K. Nowotny, and L. Sheppard, "Titanium dioxide for solar-hydrogen. I. functional properties," Int. J. Hydr. Energ. 32, 2609 - 2629 (2007). [CrossRef]
• J. Nowotny, T. Bak, M. K. Nowotny, and L. Sheppard, "Titanium dioxide for solar-hydrogen. III. kinetic effects," Int. J. Hydr. Energ. 32, 2644-2650 (2007). [CrossRef]
• J. Nowotny, T. Bak, M. K. Nowotny, and L. Sheppard, "Titanium dioxide for solar-hydrogen. IV. collective and local factors in photolysis of water," Int. J. Hydr. Energ. 32, 2651-2659 (2007). [CrossRef]

J. Alloys Compounds

• W. A. Badawy, "Effect of porous silicon layer on the performance of Si/oxide photovoltaic and photoelectrochemical cells," J. Alloys Compounds 464, 347-351 (2008). [CrossRef]

J. Am. Chem. Soc.

• R. Nakamura and Y. Nakato, "In situ FTIR studies of primary intermediates of photocatalytic reactions on nanocrystalline TiO2 films in contact with aqueous solutions," J. Am. Chem. Soc. 126, 1290-1298 (2004). [CrossRef] [PubMed]
• R. Nakamura, T. Okamura, N. Ohashi, A. Imanishi, and Y. Nakato, "Molecular mechanisms of photoinduced oxygen evolution, PL emission, and surface roughening at atomically smooth (110) and (100) n-TiO2 (rutile) surfaces in aqueous acidic solutions," J. Am. Chem. Soc. 127, 12975-12983 (2005). [CrossRef] [PubMed]
• Y. Tian and T. Tatsuma, "Mechanismsand applications of plasmon-induced charge separationat tio2 films loaded with gold nanoparticles," J. Am. Chem. Soc. 127, 7632-7637 (2005). [CrossRef] [PubMed]
• K. Ueno, S. Juodkazis, V. Mizeikis, K. Sasaki, and H. Misawa, "Spectrally-resolved atomic-scale variations of gold nanorods," J. Am. Chem. Soc. 128, 14226-14227 (2006). [CrossRef] [PubMed]
• Y. Tian and T. Tatsuma, "Mechanisms and applications of plasmon-induced charge separation at TiO2 films loaded with gold nanoparticles," J. Am. Chem. Soc. 127, 7632-7637 (2005). [CrossRef] [PubMed]
• M. K. Nazeeruddin, P. Pechy, T. Renouard, S. M. Zakeeruddin, R. Humpry-Baker, P. Comte, P. Liska, L. Cevey, E. Costa, V. Shklover, L. Spiccia, G. B. Deacon, C. A. Bignozzi, and M. Grätzel, "Engineering efficient panchromatic sensitizers for nanocrystalline TiO2-based solar cells," J. Am. Chem. Soc. 123, 1613 - 1624 (2001). [CrossRef] [PubMed]

J. Appl. Phys.

• S. Pillipai, K. R. Catchpole, T. Trupke, and M. A. Green, "Surface plasmon enhanced silicon solar cells," J. Appl. Phys. 101, 093105 (2007). [CrossRef]

J. Electrochem. Soc.

• C. Gutierrez and P. Salvador, "Mechanisms of competitive photoelectrochemical oxidation of I and H2O at nTiO2 electrodes: A kinetic approach," J. Electrochem. Soc. 133, 924 - 929 (1986). [CrossRef]

J. Mater. Chem.

• T. Hasobe, H. Imahori, S. Fukuzumi, and P. V. Kamat, "Nanostructured assembly of porphyrin clusters for light energyconversion," J. Mater. Chem. 13, 2515-2520 (2003). [CrossRef]

J. Nanophoton.

• Y. Yokota, K. Ueno, V. Mizeikis, S. Juodkazis, K. Sasaki, and H. Misawa, "Optical characterization of plasmonic metallic nanostructures fabricated by high-resolution lithography," J. Nanophoton. 1, 011594 (2008). [CrossRef]

J. Nanosci. Nanotechnol.

• V. Mizeikis, E. Kowalska, and S. Juodkazis, "Resonant localization, enhancement, and polarization of optical fields in nano-scale interface regions for photo-catalytic applications," J. Nanosci. Nanotechnol.2010 (in press).

J. Phys. Chem. C

• P. Salvador and C. Gutierrez, "The nature of surface states involved in the photo- and electroluminescence spectra of n-titanium dioxide electrodes," J. Phys. Chem. C 84, 3696 - 3698 (1984).
• H. Imahori and T. Umeyama, "Donor-acceptor nanoarchitecture on semiconducting electrodes forsolar energy conversion," J. Phys. Chem. C 113, 9029-9039 (2009). [CrossRef]
• P. Salvador, "Kinetic approach to the photocurrent transients in water photoelectrolysis at n-titanium dioxide electrodes. 1. analysis of the ratio of the instantaneous to steady-state photocurrent," J. Phys. Chem. C 89, 3683-3869 (1985).
• P. V. Kamat, "Meeting the clean energy demand: Nanostructure architectures for solar energy conversion," J. Phys. Chem. C 111, 2834-2860 (2007). [CrossRef]
• T. Tachikawa, M. Fujitsuka, and T. Majima, "Mechanistic insight into the TiO2 photocatalytic reactions: design of new photocatalysts," J. Phys. Chem. C 111, 5259- 5275 (2007). [CrossRef]

J. Power Sources

• M. Radecka, M. Rekas, A. Trenczek-Zajac, and K. Zakrzewska, "Importance of the band gap energy and flat band potential for application of modified TiO2 photoanodes in water photolysis," J. Power Sources 181, 46-55 (2008). [CrossRef]

J. Sol. Stat. Electrochem.

• J. Juodkazyt?, B. Šebeka, P. Kalinauskas, and K. Juodkazis, "Light energy accumulation using Ti/RuO2 electrode as capacitor," J. Sol. Stat. Electrochem. 14, 741 - 746 (2010). [CrossRef]
• K. Juodkazis, J. Juodkazyt?, R. Vilkauskait?, and V. Jasulaitien?, "Nickel surface anodic oxidation and electrocatalysis of oxygen evolution," J. Sol. Stat. Electrochem. 12, 1469 - 1479 (2008). [CrossRef]
• K. Juodkazis, J. Juodkazyt?, V.  Šukien?, A . Grigucevi?ien?, and A . Selskis, "On the charge storage mechanism at RuO2/0.5 M H2SO4 interface," J. Sol. Stat. Electrochem. 12, 1399 - 1404 (2008). [CrossRef]

Jpn. J. Appl. Phys.

• S. Juodkazis, A. Yamaguchi, H. Ishii, S. Matsuo, H. Takagi, and H. Misawa, "Photo-electrochemical deposition of platinum on TiO2 with resolution of tens-of-nm by using a mask elaborated with electron-beam lithography," Jpn. J. Appl. Phys. 40, 4246-4251 (2001). [CrossRef]

Lith. J. Phys.

• K. Juodkazis, J. Juodkazyt?, Y. Tabuchi, S. Juodkazis, S. Matsuo, and H. Misawa, "Deposition of platinum and irridium on Ti surface using femtosecond laser and electrochemical activation," Lith. J. Phys. 43, 209-216 (2003).

Nature

• Z. Zou, J. Ye, K. Sayama, and H. Arakawa, "Direct splitting of water under visible light irradiation with an oxide semiconductor photocatalyst," Nature 414, 625-627 (2001). [CrossRef] [PubMed]
• A. Fujishima and K. Honda, "Electrochemical photolysis of water at a semiconductor electrode," Nature 238, 37- 38 (1972). [CrossRef] [PubMed]
• M. Grätzel, "Photoelectrochemical cells," Nature 414, 338- 344 (2001). [CrossRef] [PubMed]

Opt. Express

• S. A. Maier, "Plasmonic field enhancement and SERS in the effective mode volume picture," Opt. Express 14, 1957-1964 (2006). [CrossRef] [PubMed]

Opt. Lett.

• K. Ueno, V. Mizeikis, S. Juodkazis, K. Sasaki, and H. Misawa, "Optical properties of nano-engineered gold blocks," Opt. Lett. 30, 2158 - 2160 (2005). [CrossRef] [PubMed]

Org. Electron.

• J. Lee, J. Park, J. Kim, D. Lee, and K. Cho, "High efficiency polymer solar cells with wet deposited plasmonic gold nanodots," Org. Electron. 10, 416-420 (2009). [CrossRef]

Phys. Today

• T. W. Murphy, Jr., "Home photovoltaic systems for physicists," Phys. Today, 42- 47 (2008). [CrossRef]
• G. W. Crabtree and N. S. Lewis, "Solar energy conversion," Phys. Today 60, 37 - 42 (2007). [CrossRef]

Powder Technol.

• C. Chou, R. Yang, C. Yeh, and Y. Lin, "Preparation of tio2/nano-metal composite particles and thier applications in dye-sensitized solar cells," Powder Technol. 194, 95-105 (2009). [CrossRef]

Prog. Photovolt.

• M. A. Green, K. Emery, Y. Hishikawa, and W. Warta, "Solar cell efficiency tables (version 31)," Prog. Photovolt. 16, 61 - 67 (2008). [CrossRef]

Renew. Sustain. Ener. Rev.

• M. Ni, M. K. H. Leung, D. Y. Leung, and K. Sumathy, "A review and recent developments in photocatalytic water splitting using TiO2 for hydrogen production," Renew. Sustain. Ener. Rev. 11, 401-425 (2007). [CrossRef]

Solar Ener. Mat. Solar Cells

• G. K. Mor, O. K. Varghese, M. Paulose, K. Shankar, and C. A. Grimes, "A review on highly-ordered TiO2 nanotube-arrays: fabrication, material properties, and solar energy applications," Solar Ener. Mat. Solar Cells 90, 2011 - 2075 (2006). [CrossRef]

Solar Energ. Mat. Solar Cells

• E. L. Miller, D. Paluselli, B. Marsen, and R. E. Rocheleau, "Development of reactively sputtered metal oxide films for hydrogen-producing hybrid multijunction photoelectrodes," Solar Energ. Mat. Solar Cells 88(2), 131-144 (2005). [CrossRef]
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Solar Energy

• V. M. Aroutiounian, V. M. Arakelyan, and G. E. Shahnazaryan, "Metal oxide photoelectrodes for hydrogen generation using solar radiation-driven water splitting," Solar Energy 78, 581 - 592 (2005). [CrossRef]

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Thin Solid Films

• N. Dhere and A. H. Jahagirdar, "Photoelectrochemical water splitting for hydrogen production using combination of CIGS2 solar cell and RuO2 photocatalyst," Thin Solid Films 480-481, 462-465 (2005). [CrossRef]

Transact. Inst. of Metal Finishing

• J. Juodkazyt?, R. Vilkauskait?, B. Šebeka, and K. Juodkazis, "Difference between surface electrochemistry of ruthenium and RuO2 electrodes," Transact. Inst. of Metal Finishing 85, 194 - 201 (2007). [CrossRef]

Other

• D. Dobos, Electrochemical Data (Mir, Moscow, 1980).
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• Comparison of photon energy with potential E0 = 1.23 V. According to ?G = ?nFE0, where G represents the isobaric-isothermal potential (Gibbs energy) of the reaction or the chemical potential of the substance, n is the number of electrons, and F is the Faraday constant, in the case of formation of water molecule H2 + ½O2 = H2O, one would find: ?G = ?2×96500×1.23 = ?2.37390×105 (J mol?1). As there are two H-O bonds in H2O molecule, the energy corresponding to one bond is 18695 J mol?1 or 7.409×1023 eV mol?1. Division of the latter value by Avogadro number NA = 6.02×1023, gives the energy of one chemical bond, 1.23 eV. This is the minimum photon energy required to break the bond between H and O in H2O molecule.
• L. Han, A. Islam, N. Koide, and R. Yamanaka, "Alternative technology enables large-area solar-cell production," SPIE Newsroom, doi: 10.1117/2.1200908.1774 (2009). [CrossRef]

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