Direct Hydrogen Evolution from Saline Water Reduction at Neutral pH using Organic Photocathodes

Haro, Marta; Solis, Claudia Alejandra; Blas‐Ferrando, Vicente M.; Margeat, Olivier; Dhkil, Sadok Ben; Videlot‐Ackermann, Christine; Ackermann, Jörg; Fonzo, Fabio Di; Guerrero, Antonio; Giménez, Sixto

doi:10.1002/cssc.201600961

Cited by 18 publications

(15 citation statements)

References 27 publications

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“…179,180 The delamination/disruption is instead not observed in our HSL-free photocathodes, in agreement with previous studies. [75][76][77][78][79][80][81][82][83][84][85] Stabilizing strategies The decrease of the photocurrents observed during the potentiostatic stability test pointed out the need to implement stabilizing strategies to improve the endurance of the as-prepared photoelectrodes. Both Pt detachment/dissolution and delamination/disruption of the layered structure of the photocathodes based on GO and RGO can be at the origin of the performances degradation.…”

Section: Photoelectrochemical Characterizationmentioning

confidence: 99%

“…104 While TiO 2 and its sub-stoichiometric phases have demonstrated to be consolidated ESL materials, [80][81][82][83]85 the choice for the HSL counterpart has been a more complex task. In fact, although efficient HSL materials have been identified (e.g., MoO 3 , 77 WO 3 , 82 NiO, 80 CuI, 83,85 PEDOT:PSS [75][76][77][78][79][80][81] ) their intrinsic electrochemical degradation under HER-working conditions limited the lifetime of the photocathodes, lasting from several minutes to about few hours (up to 10 hours in the case of WO 3 ). [75][76][77][78][79][80][81][82][83][84][85] Moreover, the operational activity of the most efficient structures has been demonstrated only in acidic conditions, [76][77][78][79][80][81][82][83][84][85] with only a few examples showing remarkable cathodic J 0V vs RHE of 1.2 mA cm -2 at neutral pH.…”

Section: Introductionmentioning

confidence: 99%

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Graphene-Based Hole-Selective Layers for High-Efficiency, Solution-Processed, Large-Area, Flexible, Hydrogen-Evolving Organic Photocathodes

et al. 2017

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Regio-regular poly(3-hexylthiophene-2,5-diyl) (rr-P3HT), the work-horse of organic photovoltaics, has been recently exploited in bulk heterojunction (BHJ) configuration with phenyl-C61-butyric acid methyl ester (PCBM) for solution-processed hydrogen-evolving photocathodes, reaching cathodic photocurrents at 0 V vs. RHE (J 0V vs RHE ) of up to 8 mA cm -2 . The photoelectrochemical performance of these photocathodes strongly depends on the presence of the electron (ESL) and hole (HSL) selective layer. While TiO 2 and its sub-stoichiometric phases are consolidated ESL materials, the currently used HSLs (e.g., MoO 3 , CuI, PEDOTT:PSS, WO 3 ) suffer electrochemical degradation under hydrogen evolution reaction (HER)-working conditions. In this work, we use solution-processed graphene derivatives as HSL to boost efficiency and durability of rr-P3HT:PCBM-based photocathodes, demonstrating record-high performance. In fact, our devices show cathodic J 0V vs RHE of 6.01 mA cm -2 , onset potential (V o ) of 0.6 V vs. RHE, ratiometric power-saved efficiency (φ saved ) of 1.11% and operational activity of 20 hours in 0.5 M H 2 SO 4 solution. Moreover, the designed photocathodes are effectively working in different pH environments ranging from acid to basic. This is pivotal for their exploitation in tandem configurations, where photoanodes operate only in restricted electrochemical conditions. Furthermore, we demonstrate the scalability of our all-solution processed approach by fabricating a large-area (~9 cm 2 ) photocathode on flexible substrate, achieving remarkable cathodic J 0V vs RHE of 2.8 mA cm -2 , V o of 0.45 V vs. RHE and φ saved of 0.31%. This is the first demonstration of highefficient rr-P3HT:PCBM flexible photocathodes based on low-cost and solution-processed manufacturing techniques.

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Section: Photoelectrochemical Characterizationmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Graphene-Based Hole-Selective Layers for High-Efficiency, Solution-Processed, Large-Area, Flexible, Hydrogen-Evolving Organic Photocathodes

et al. 2017

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“…PbS photo-oxidation caused by the increase of the oxide species modifying the redox potential of the reaction according to Nernst equation, subsequently leading to a competition between OER and PbS oxidation at certain concentration. [46] After 100 voltammetry scans under illumination, the PbS/BiVO4 CV is not anymore evolving, indicating reversible changes in the photoanode between two oxide states of PbOx. The evolution of the CV during these 100 scans is shown in Supporting Information, Figure S17.…”

Section: Resultsmentioning

confidence: 97%

Lead Sulfide Nanocubes for Solar Energy Storage

et al. 2020

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PbS nanocubes have been produced by a very simple solvothermal procedure that employs a unique molecule, ethylenediamine, as solvent and capping ligand to control the size and shape of nanocrystals. Detailed structural, optical and photoelectrochemical evaluation confirmed the suitability of these nanoparticles for photocapacitive applications, when synergistically combined with spin-coated BiVO4 photoelectrodes, as derived from the estimated energy diagram. Furthermore, the p-n junction facilitates the photo-oxidation of PbS nanoparticles under light irradiation. In the dark, the photogenerated charges are released providing an electric output response with a solar-to-current efficiency of 0.042 %, storing energy extra to the H2 produced by water splitting when the BiVO4 photoanode works under illumination. This study highlights the importance of the synthetic route and methodology to ensemble materials for advanced solar energy storage applications.

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“…Compared to HTLs, the development of materials for the ETL is less advanced. Although C 60 and Al:ZnO (AZO) as ETLs demonstrated some improvement in the performance of BHJ photocathodes, the photocurrent was observed to quickly decay due to the instability of C 60 and AZO in acid water . By contrast, given its excellent aqueous stability, large bandgap energy, and effective ability for electron transport, the most effective ETL material so far demonstrated is titanium oxide.…”

Section: Direct Water Splitting From Organic Semiconductor Pec Cellsmentioning

confidence: 99%

Organic Semiconductor Based Devices for Solar Water Splitting

Yao

Rahmanudin

Guijarro

et al. 2018

Advanced Energy Materials

102

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transforms electrical energy into mole cular hydrogen (H 2 ) and oxygen (O 2 ) that can be reconverted into electrical energy on demand with a fuel cell, represents a leading approach for the scalable long term storage and transport of renewable energy, [4] given the terrestrial abundance of H 2 O. Considering that H 2 is also an essential chemical building block (e.g., for NH 3 production) and can also be converted into liquid fuels with CO 2 using industri ally established transformations (reverse water-gas shift and Fischer-Tropsch), an energy and chemical economy based pri marily on hydrogen produced from solar energy is not only conceivable, but highly anticipated. However, to attain economi callyfeasible solardriven H 2 production at a global scale, challenges remain in the identification of materials and systems that can achieve high solartofuel energy conversion efficiency and robust perfor mance at lowcost. [5] In particular, the development of suitable light harvesting semiconducting materials with ideal properties for solardriven water split ting has been a major focus of research in the past decades. [6] To date, although numerous inorganic semiconductors [7][8][9][10][11][12] have demonstrated solar watersplitting in various device architectures, [13] systems that can produce H 2 at a price competitive with fossil fuel based H 2 production remain elusive. [14] Therefore, a new generation of high performance, stable materials based on earth abundant elements and low cost processing is needed to enable solar water splitting for the glo balized storage of solar energy and a carbonneutral industrial chemical economy.Solutionprocessed organic semiconductors, which con tain an aromatic core of conjugated carbon-carbon bonds, which brings an electronic structure suitable for semicon ducting operation, and flexible appendages (e.g., alkyl groups) to afford solubility in common solvents, represent a promising class of materials to enable lowcost, high performance solar fuel production. Indeed, both conjugated polymers and small molecules have already been wellestablished in organic photo voltaic (OPV) devices. [15][16][17][18][19][20] The solartoelectricity (photovoltaic) power conversion efficiency (η PV ) of stateofthe art OPVs has surpassed 17% by optimization of the organic semiconductor molecular structures and device engineering. [21][22][23][24] Considering the success of solutionprocessable organic semiconductors in OPV, research is now emerging to exploit their advantages over Solution processable organic semiconductors are well-established as highperformance materials for inexpensive and scalable solar energy conversion in organic photovoltaic (OPV) devices, but their promise in the economic conversion of solar energy into chemical energy (solar fuels) has only recently been recognized. Herein, the main approaches employing organic semiconductor-based devices toward solar H 2 generation via water splitting are compared and performance demonstrations are reviewed. OPV-biased water electrolysis is see...

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Direct Hydrogen Evolution from Saline Water Reduction at Neutral pH using Organic Photocathodes

Cited by 18 publications

References 27 publications

Graphene-Based Hole-Selective Layers for High-Efficiency, Solution-Processed, Large-Area, Flexible, Hydrogen-Evolving Organic Photocathodes

Graphene-Based Hole-Selective Layers for High-Efficiency, Solution-Processed, Large-Area, Flexible, Hydrogen-Evolving Organic Photocathodes

Lead Sulfide Nanocubes for Solar Energy Storage

Organic Semiconductor Based Devices for Solar Water Splitting

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