Visible Light-Driven Water Splitting in Photoelectrochemical Cells with Supramolecular Catalysts on Photoanodes

Ding, Xin; Gao, Yan; Zhang, Linlin; Yu, Ze; Liu, Jianhui; Sun, Licheng

doi:10.1021/cs500518k

Cited by 116 publications

(92 citation statements)

References 26 publications

(47 reference statements)

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“…[13][14][15] In the last decade several systems have been proposed employing either metal oxide nanoparticles 8,[16][17][18][19][20][21][22][23][24] or molecular complexes 8,[25][26][27][28] as water oxidation catalyst (WOC). Furthermore, the coupling between the WOC, the chromophore and an electron accepting semiconductor into a photoanode has been achieved through co-absorption of both the catalyst and the chromophore 16,[29][30][31][32] or through dye-WOC supramolecular complexes. [33][34][35][36] Acquiring a fundamental understanding of the electron transfer processes and catalytic water oxidation mechanism following light excitation of the photoanode is essential for the design and the optimization of solar fuel cells.…”

Section: Introductionmentioning

confidence: 99%

A Dynamic View of Proton-Coupled Electron Transfer in Photocatalytic Water Splitting

et al. 2016

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Section: Introductionmentioning

confidence: 99%

A Dynamic View of Proton-Coupled Electron Transfer in Photocatalytic Water Splitting

et al. 2016

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“…It, however, requires a fine regulation of photon, electron and proton management between both photocatalytic systems, which can be achieved through the grafting of the active components at the surface of transparent conductive electrode substrates [22]. Extending the n-type dye-sensitized solar cell (DSSC) technology, significant achievements in this direction have been reported recently regarding the preparation of molecular-based photoanodes for water oxidation [23][24][25][26][27][28][29]. Co-grafting of a water-oxidizing catalyst with a molecular dye on mesoscopic TiO 2 substrates yielded electrodes able to deliver up to 2 mA cm 22 photocurrent corresponding to O 2 evolution under visible irradiation [27].…”

Section: Introductionmentioning

confidence: 99%

Dye-sensitized PS- b -P2VP-templated nickel oxide films for photoelectrochemical applications

et al. 2015

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Moving from homogeneous water-splitting photocatalytic systems to photoelectrochemical devices requires the preparation and evaluation of novel p-type transparent conductive photoelectrode substrates. We report here on the sensitization of polystyrene-block-poly-(2-vinylpyridine) (PS-b-P2VP) diblock copolymer-templated NiO films with an organic push -pull dye. The potential of these new templated NiO film preparations for photoelectrochemical applications is compared with NiO material templated by F108 triblock copolymers. We conclude that NiO films are promising materials for the construction of dye-sensitized photocathodes to be inserted into photoelectrochemical (PEC) cells. However, a combined effort at the interface between materials science and molecular chemistry, ideally funded within a Global Artificial Photosynthesis Project, is still needed to improve the overall performance of the photoelectrodes and progress towards economically viable PEC devices.

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“…In a DSPEC, visible light is absorbed by a chromophore, initiating a series of events that culminate in water splitting: injection, intraassembly electron transfer, catalyst activation, and electron transfer to a cathode or photocathode for H 2 production. Sun and coworkers have recently demonstrated visible-light-driven water splitting with a coloading approach combining Ru(II) polypyridyl-based light absorbers and catalysts on TiO 2 (9). The efficiency of DSPEC devices is dependent on interfacial dynamics and competing kinetic processes.…”

mentioning

confidence: 99%

Visible photoelectrochemical water splitting into H ₂ and O ₂ in a dye-sensitized photoelectrosynthesis cell

Alibabaei

Sherman

Norris

et al. 2015

Proc. Natl. Acad. Sci. U.S.A.

141

163

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A hybrid strategy for solar water splitting is exploited here based on a dye-sensitized photoelectrosynthesis cell (DSPEC) with a mesoporous SnO 2 /TiO 2 core/shell nanostructured electrode derivatized with a surface-bound Ru(II) polypyridyl-based chromophore-catalyst assembly. The assembly, [(4, H 2 ) 2 bpy) 2 Ru(4-Mebpy-4'-bimpy)Ru (tpy) (OH 2 dye-sensitized photoelectrosynthesis cell | water oxidation | core/shell A lthough promising, significant challenges remain in the search for successful strategies for artificial photosynthesis by water splitting into oxygen and hydrogen or reduction of CO 2 to reduced forms of carbon (1-5). In a dye-sensitized photoelectrosynthesis cell (DSPEC), a wide band gap, nanoparticle oxide film, typically TiO 2 , is derivatized with a surface-bound molecular assembly or assemblies for light absorption and catalysis (6-8). In a DSPEC, visible light is absorbed by a chromophore, initiating a series of events that culminate in water splitting: injection, intraassembly electron transfer, catalyst activation, and electron transfer to a cathode or photocathode for H 2 production. Sun and coworkers have recently demonstrated visible-light-driven water splitting with a coloading approach combining Ru(II) polypyridyl-based light absorbers and catalysts on TiO 2 (9). The efficiency of DSPEC devices is dependent on interfacial dynamics and competing kinetic processes. A major limiting factor is the requirement for accumulating multiple oxidative equivalents at a catalyst site to meet the 4e − /4H + demands for oxidizing water to dioxygen (2H 2 O -4e − -4H + → O 2 ) in competition with back electron transfer of injected electrons to the oxidized assembly.One approach to achieving structural control of local electron transfer dynamics at the oxide interface in dye-sensitized devices is by use of nanostructured core/shell electrodes (10-12). In this approach, a mesoporous network of nanoparticles is uniformly coated with a thin oxide overlayer prepared by atomic layer deposition (ALD). We have used core/shell electrodes to demonstrate benzyl alcohol dehydrogenation (13). This approach has also been used to enhance the efficiency of dye-sensitized solar cells (14,15). Recently, we described the use of a core/shell consisting of an inner core of a nanoparticle transparent conducting oxide, tin-doped indium oxide (nanoITO), and a thin outer shell of TiO 2 for water splitting by visible light (16 Fig. 1A, provided the basis for a photoanode in a DSPEC application with a Pt cathode for H 2 generation with a small applied bias in an acetate buffer at pH 4.6.Application of the core/shell structure led to a greatly enhanced efficiency for water splitting compared with mesoscopic, nanoparticle TiO 2 but the per-photon absorbed efficiency of the resulting DSPEC was relatively low and problems arose from longterm instability due to loss of the assembly from the oxide surface in the acetate buffer at pH 4.6. The latter is problematic because the rate of water oxidation is enhanced by added buffer bases...

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Visible Light-Driven Water Splitting in Photoelectrochemical Cells with Supramolecular Catalysts on Photoanodes

Cited by 116 publications

References 26 publications

A Dynamic View of Proton-Coupled Electron Transfer in Photocatalytic Water Splitting

A Dynamic View of Proton-Coupled Electron Transfer in Photocatalytic Water Splitting

Dye-sensitized PS- b -P2VP-templated nickel oxide films for photoelectrochemical applications

Visible photoelectrochemical water splitting into H ₂ and O ₂ in a dye-sensitized photoelectrosynthesis cell

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Visible Light-Driven Water Splitting in Photoelectrochemical Cells with Supramolecular Catalysts on Photoanodes

Cited by 116 publications

References 26 publications

A Dynamic View of Proton-Coupled Electron Transfer in Photocatalytic Water Splitting

A Dynamic View of Proton-Coupled Electron Transfer in Photocatalytic Water Splitting

Dye-sensitized PS- b -P2VP-templated nickel oxide films for photoelectrochemical applications

Visible photoelectrochemical water splitting into H 2 and O 2 in a dye-sensitized photoelectrosynthesis cell

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Visible photoelectrochemical water splitting into H ₂ and O ₂ in a dye-sensitized photoelectrosynthesis cell