Artificial Molecular Photosynthetic Systems: Towards Efficient Photoelectrochemical Water Oxidation

Yamamoto, Masanori; Tanaka, Koji

doi:10.1002/cplu.201600236

Cited by 42 publications

(50 citation statements)

References 130 publications

(319 reference statements)

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“…1 This process occurs at the CaMn 4 O 4 oxygen evolving complex (OEC) upon the accumulation of four oxidizing equivalents in a single turnover, 2 a strategy that minimizes extra energy input (overpotential) 3 and avoids the formation of partially oxidized product(s) (e.g. H 2 O 2 ).…”

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confidence: 99%

Catalytic Water Oxidation by a Bio-inspired Nickel Complex with a Redox-Active Ligand

Wang

Bruner

2017

Inorg. Chem.

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The oxidation of water to dioxygen is important in natural photosynthesis. One of nature’s strategies for managing such multi-electron transfer reactions is to employ redox active metal-organic cofactor arrays. One prototype example is the copper-tyrosinate active site found in galactose oxidase. In this work, we have implemented such a strategy to develop a bio-inspired nickel-phenolate complex capable of catalyzing the oxidation of water to O2 electrochemically at neutral pH with a modest overpotential. The employment of the redox-active ligand turned out to be a useful strategy to avoid the formation of high-valent nickel intermediates while a reasonable turnover rate (0.15 s−1) is retained.

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confidence: 99%

Catalytic Water Oxidation by a Bio-inspired Nickel Complex with a Redox-Active Ligand

Wang

Bruner

2017

Inorg. Chem.

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“…[162] Since that report, a variety of molecular water oxidation catalysts, based on Ru, Ir, and other earth-abundant elements have been reported. [13,14,24] Typically, the catalysts were coupled with organic light absorbers (mainly based on noble metals) for water oxidation leading to poor light absorption and stability. The use of semiconductors, that absorb over a broad spectral range with high photostabilities, are preferred compared to organic dyes.…”

Section: Noble-metal Molecular Catalystsmentioning

confidence: 99%

“…It was based on TiO 2 as a photoanode for generating O 2 and Pt as a counter electrode for generating H 2 11. Their research led to an extended series of research efforts devoted to the development of high‐efficiency PEC systems for water splitting 12–16…”

Section: Introductionmentioning

confidence: 99%

“…[11] Their research led to an extended series of research efforts devoted to the development of high-efficiency PEC systems for water splitting. [12][13][14][15][16] The past few decades have seen the rapid development of PEC water splitting systems, including both semiconductor sensitized systems [12,17] and organic dye sensitized systems. [13,14,18] Among them, semiconductor sensitized systems have been widely investigated due to ease of preparation of semiconductors, good stability, broad spectral response, and relatively low cost.…”

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confidence: 99%

“…[12][13][14][15][16] The past few decades have seen the rapid development of PEC water splitting systems, including both semiconductor sensitized systems [12,17] and organic dye sensitized systems. [13,14,18] Among them, semiconductor sensitized systems have been widely investigated due to ease of preparation of semiconductors, good stability, broad spectral response, and relatively low cost. However, it is intrinsically difficult to directly employ semiconductor electrodes for highly efficient and stable PEC water splitting because of the challenges faced, including: inhibiting electron-hole recombination, accelerating poor interfacial charge transfer, matching energy levels for feasible water redox reactions, and narrowing bandgaps for broad sunlight absorption, all to be integrated simultaneously.…”

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confidence: 99%

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Hybrid Photoelectrochemical Water Splitting Systems: From Interface Design to System Assembly

Niu

Wang

et al. 2019

Advanced Energy Materials

189

120

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Photoelectrochemical (PEC) water splitting has attracted increasing attention due to its potential to mitigate energy and environmental issues. Hybrid PEC systems containing semiconductor photosensitizers and molecular catalysts are reported to be highly active and stable for water splitting with great potential for facilitating clean fuels production. In this review, following a showcasing of the fundamental details of hybrid PEC systems for water splitting, semiconductor/molecular catalyst interface designs are highlighted, with a focus on interfacial physicochemical interactions and binding, and interfacial energetics and dynamics for efficient charge transfer. Recent advances in hybrid system assemblies for PEC water splitting are also briefly introduced. Finally, future challenges and directions in the field of hybrid PEC water splitting for solar energy conversion are reviewed. The current review provides state‐of‐the‐art strategies for optimized interface design for creating highly active and stable PEC water splitting assemblies.

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Förster Resonance Energy Transfer in Linear DNA Multifluorophore Photonic Wires: Comparing Dual versus Split Rail Building Block Designs

Cunningham

Spillmann

Melinger

et al. 2021

Advanced Optical Materials

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DNA scaffolds provide a means to precisely organize chromophores into large biomimetic exciton networks and direct energy transport for nanoscale sensing and light‐harvesting applications. Here, a functional building block of minimal complexity that maximizes the Förster resonance energy transfer (FRET) efficiency is sought. Using a model system consisting of three FRET steps in a 4‐dye cascade: Cy3→Cy3.5→Cy5→Cy5.5, we evaluate how this building block employs multiple interacting versus redundant FRET pathways. Variants of a dual rail design, where one or two copies of each dye are aligned in rigid linear parallel rows, are compared to a split rail format, where varying degrees of spacing are introduced between the rows. The FRET processes are assessed via steady‐state, time‐resolved, and single‐molecule spectroscopy. Experiments and simulation reveal the dual rail design as more efficient than the split rail and suggest the design principle that efficient FRET networks must balance the increase in FRET rate from multiple interacting pathways with undesirable fluorescence quenching between dyes in close proximity. Hybrid fluorophore combinations are identified as a strategy to mitigate this quenching, leading to optimized dual rails capable of 50% end‐to‐end efficiency. These insights can help guide the design of functional photonic wires based on DNA scaffolds.

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Artificial Molecular Photosynthetic Systems: Towards Efficient Photoelectrochemical Water Oxidation

Cited by 42 publications

References 130 publications

Catalytic Water Oxidation by a Bio-inspired Nickel Complex with a Redox-Active Ligand

Catalytic Water Oxidation by a Bio-inspired Nickel Complex with a Redox-Active Ligand

Hybrid Photoelectrochemical Water Splitting Systems: From Interface Design to System Assembly

Förster Resonance Energy Transfer in Linear DNA Multifluorophore Photonic Wires: Comparing Dual versus Split Rail Building Block Designs

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