Dye-Sensitized Hydrobromic Acid Splitting for Hydrogen Solar Fuel Production

Brady, Matthew D.; Sampaio, Renato N.; Wang, Degao; Meyer, Thomas J.; Meyer, Gerald J.

doi:10.1021/jacs.7b09367

Cited by 71 publications

(76 citation statements)

References 34 publications

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“…It can be understood that the photogenerated electrons transfer from TiO 2 to PMo 12 to form a saturated electron PMo 12 (HPB). This process produced negative current . After the electrons of PMo 12 are reached to the saturation, the PMo 12 (HPB) (absorbing visible light) and TiO 2 (absorbing ultraviolet light) will be simultaneously excited by the continuous illumination, so that the excited electrons are conducted to the external circuit to form a positive photocurrent and the photocurrent intensity is increased gradually over time, until reached the stable current.…”

Section: Resultsmentioning

confidence: 99%

A Strategy to Obtain Long‐Term Stable Heteropoly Blues for Photosensitive Property Investigations

Chen

et al. 2018

Advanced Optical Materials

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which should have wide spectrum absorptions, anchoring groups, and appropriate energy levels in order to absorb more sunlight and excite the ground-state electrons to the excited state, then inject into the semiconductor conduction band, while the holes remain in the dye molecule form the charge separations, which ensure the effective regenerations of the photosensitizers and the unidirectional electron injections. [2] In recent decades, great efforts have been made to develop the photosensitizers with high stability, low-cost, and high solar energy conversion in the fields of photocatalysts and solar cells. [3,4] However, developing broad-spectrum photosensitizers is still a big challenge. At present, the commonly used photosensitizers including ruthenium-pyridine, porphyrin, and pure organic dyes, have efficiently improved the power conversion efficiencies (PCEs) of the DSSCs. [5] However, their large-scale productions and applications in photovoltaic industry have been limited by their high costs and the cumbersome process in the synthesis and purification of photosensitizers. [6] Furthermore, the defects of some photosensitizers in spectral absorption also restrict the utilization of sunlight. So, it is urgent to develop the photosensitizers with environment-friendly, simple preparations, low costs, and wide spectra absorptions.Heteropoly blues (HPBs) is a reductive state of polyoxometalates (POMs representing oxidation state) with fascinating structures, abundant element compositions, reversible redox properties, and wide pH stability. [7,8] The advantages of HPBs as photosensitizer are as follows: i) their wide and strong spectral absorptions in visible and near-IR regions; ii) the anchoring groups are easily to coordinated to HPBs to firmly adsorb on the semiconductor surface; iii) their energy levels involving the lowest unoccupied molecular orbital (LUMO) and the highest occupied molecular orbital (HOMO) can be adjusted by the composition, structure, and charge density to ensure the effective unidirectional electron injections and photosensitizer regenerations; [9] iv) their excellent light, thermal and electrochemical stability, their ability to accept or lose "blue" electrons without any structural transformations. As a kind of the potential photosensitizer candidates, HPBs have been increasingly recognized in terms of photocatalysis and solar cells. [10][11][12][13][14] However, the instability of HPBs in the air restricts the further research of their photosensitivity and their use as the photosensitizers in DSSCs.The photosensitizer is the soul of dye-sensitized solar cells (DSSCs), i.e., the key factor influencing the performance of DSSCs. The commonly used photo sensitizers are expensive carboxylic pyridine ruthenium-based complexes, so it is urgent to develop low-cost photosensitizers. Heteropoly blues (HPBs) could be a kind of excellent photosensitizers due to their wide spectra absorption; however, most of them are hardly stable in the air. Here, a strategy of combining the improved vacuum...

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Section: Resultsmentioning

confidence: 99%

A Strategy to Obtain Long‐Term Stable Heteropoly Blues for Photosensitive Property Investigations

Chen

et al. 2018

Advanced Optical Materials

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“…Besides alcohol oxidation, T. J. Meyer, G. J. Meyer, and their coworkers have also been investigating halide oxidation reactions as substitutes for water oxidation in a PEC . Water oxidation is a four‐electron process and poses many kinetic challenges, whereas halide oxidation reactions are just two‐electron processes and should in principle be faster.…”

Section: Pecs For Catalytic Synthesesmentioning

confidence: 99%

“…This homogeneous halide oxidation was followed by a paper on using a DSPEC for Br − oxidation (Figure b) . Brady et al .…”

Section: Pecs For Catalytic Synthesesmentioning

confidence: 99%

Photoelectrochemical Cells for Artificial Photosynthesis: Alternatives to Water Oxidation

Boruah

Chin

et al. 2020

ChemNanoMat

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Photoelectrochemical cells have been used as one of the most common artificial photosynthetic approaches to mimic natural photosynthetic water splitting reactions. However, despite the tremendous advances made to improve the affordability and efficiency of photoelectrochemical water splitting, it is still not an economically feasible method to produce solar fuels currently since only the H 2 evolving reduction half-reaction generates valuable fuels. Therefore, in this review, we intend to highlight other underexplored substrates and reactions for producing solar fuels in photo-electrochemical cells, as well as alternative architectures including temporally independent and biohybrid systems. We show that besides water oxidation, electrocatalytic or photoredox reactions for pollutant degradation, biomass valorization, and organic chemical synthesis can be or have been successfully adapted for photoelectrochemical cells, thus offering a virtually infinite number of possibilities for artificial photosynthetic applications which generate valuable products in both the reduction and oxidation half reactions.

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“…This concept had been pioneered by Meyer and co-workers, who demonstrated its potential for chloride [25] and benzyl alcohol oxidation with simultaneous H 2 evolution. [26] Others, including Sun and co-workers, [27][28][29][30] Meyer and co-workers, [31][32][33][34][35] Berlinguette and co-workers, [36][37][38] Reisner and co-workers, [14,[39][40][41] and Lei and co-workers, [42][43][44] have subsequently shown that the gap between AP and radical catalysis can potentially be bridged via the valorization of biomass, functionalization of amines, oxidation of other halides, photo-electrochemical reduction of CO 2 , and even photoreforming of plastics.…”

Section: Introductionmentioning

confidence: 99%

“…Cascade CC bond cleavage in macromolecular hydroxyl functionalized biodegradable(34)(35)(36) and non-biodegradable (37 and 38) polymers. In all the polymeric substrates, the sites of CC bond cleavage are highlighted in red, with multiple red colored CC bonds indicating the cascade shortening of the polymer chain.…”

mentioning

confidence: 99%

Visible Light–Driven Cascade Carbon–Carbon Bond Scission for Organic Transformations and Plastics Recycling

et al. 2019

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Significant efforts are devoted to developing artificial photosynthetic systems to produce fuels and chemicals in order to cope with the exacerbating energy and environmental crises in the world now. Nonetheless, the large-scale reactions that are the focus of the artificial photosynthesis community, such as water splitting, are thus far not economically viable, owing to the existing, cheaper alternatives to the gaseous hydrogen and oxygen products. As a potential substitute for water oxidation, here, a unique, visible light-driven oxygenation of carboncarbon bonds for the selective transformation of 32 unactivated alcohols, mediated by a vanadium photocatalyst under ambient, atmospheric conditions is presented. Furthermore, since the initial alcohol products remain as substrates, an unprecedented photodriven cascade carboncarbon bond cleavage of macromolecules can be performed. Accordingly, hydroxyl-terminated polymers such as polyethylene glycol, its block co-polymer with polycaprolactone, and even the non-biodegradable polyethylene can be repurposed into fuels and chemical feedstocks, such as formic acid and methyl formate. Thus, a distinctive approach is presented to integrate the benefits of photoredox catalysis into environmental remediation and artificial photosynthesis.

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Dye-Sensitized Hydrobromic Acid Splitting for Hydrogen Solar Fuel Production

Cited by 71 publications

References 34 publications

A Strategy to Obtain Long‐Term Stable Heteropoly Blues for Photosensitive Property Investigations

A Strategy to Obtain Long‐Term Stable Heteropoly Blues for Photosensitive Property Investigations

Photoelectrochemical Cells for Artificial Photosynthesis: Alternatives to Water Oxidation

Visible Light–Driven Cascade Carbon–Carbon Bond Scission for Organic Transformations and Plastics Recycling

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