Boosting water oxidation layer-by-layer

Hidalgo-Acosta, Jonnathan C.; Scanlon, Micheál D.; Méndez, Manuel A.; Amstutz, Véronique; Vrubel, Heron; Opałło, Marcin

doi:10.1039/c5cp06890h

Cited by 16 publications

(17 citation statements)

References 57 publications

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“…This loss of stability, which is marginal at the working conditions employed (low potentials), most likely takes place due to the swelling of the polymer and the breakdown of the electrostatic interactions binding the layers together on the electrode surface. Noticeably, all CVs in Figures A,B resemble those obtained previously in acidic aqueous media exhibiting Ir(III)‐Ir(III)/Ir(IV)‐Ir(IV) and Ir(IV)‐Ir(IV)/Ir(IV)‐Ir(V) redox transitions at 0.78 V and 1.07 V, respectively, and the onset potential for the WOR in the range 1.17–1.32 V. The formation of oxygen upon oxidation at potentials beyond this value was confirmed by gas chromatography (Supporting Information). A closer inspection of the CVs in Figure A (inset) reveals that at high water content ( X H 2 O≥0.6), the voltammetry remains practically unaffected.…”

Section: Figuresupporting

confidence: 80%

“…To achieve this, we utilized fluorinated tin oxide (FTO) electrodes modified sequentially layer‐by‐layer with the positively charged polymer poly(diallydimethylammonium chloride) (PDDA) and negatively charged citrate‐stabilized IrO 2 NPs (see Figure ). In a separate study, we clearly demonstrated the electrocatalysis of the WOR in aqueous media using these layer‐by‐layer modified FTO electrodes that exhibited good operational stability, remaining active over a wide pH‐range . Herein, these electrodes are utilized as a platform to study the electrocatalysis of the WOR in water/ACN mixtures.…”

Section: Figurementioning

confidence: 92%

“… Thus, in an effort to determine the second‐order reaction constant as accurately as possible, 20 m m HClO 4 was chosen in preference to NaHCO 3 /Na 2 SiF 6 as its slower base rate of catalysis permitted far greater temporal resolution during the kinetic study . Herein, HClO 4 was chosen 1) to have a direct comparison with the kinetic experiments previously reported, 2) as HClO 4 allows experiments to be performed without the addition of other supporting electrolytes, and 3) as the IrO 2 /PDDA bilayers on the FTO electrode exhibit optimal stability under these acidic conditions …”

Section: Figurementioning

confidence: 99%

“…−1 , 2.2 mm thickness, Solaronix) with eight bilayers of IrO 2 /PDDA. The IrO 2 NPs were synthesized and characterized as discussed previously . The catalytic electrodes were prepared using a layer‐by‐layer (LbL) methodology, sequentially depositing negatively charge citrate stabilized IrO 2 NPs and the cationic PDDA polymer.…”

Section: Figurementioning

confidence: 99%

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Enhanced Reactivity of Water Clusters towards Oxidation in Water/Acetonitrile Mixtures

et al. 2016

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[a] DedicatedtoProfessor Christian Amatore on occasion of his 65th birthdayThe water oxidationp rocess in acidified water/acetonitrile mixtures was studied by cyclic voltammetry using fluorinated tin oxide (FTO) electrodes modified layer-by-layer with deposited bilayerso fp ositivelyc harged poly(diallyldimethylammonium chloride) (PDDA) polymer andn egatively charged citrate-stabilized iridium oxide (IrO 2 )n anoparticles. The voltammetric profiles obtained at high water contents resemble those in aqueous mediaa nd remaina pproximately unchanged. However,a s the water content decreases below aw ater mole fraction (XH 2 O) of 0.6, at ipping point is reached and the onset potential for water oxidation gradually decreases. This reflects an enhanced reactivity,a nd therefore lower overpotential, of water molecules towards oxidation in water/acetonitrile mixtures. These lower kinetic barriers towards water oxidation are rationalized based on the degradation of the hydrogen bond network upon the formation of water/acetonitrile mixtures. Thus, as the ice-like structure of neat water transitions to clusters and low-bonded oligomers, these water molecules in more "free" states exhibit an enhanced susceptibility to water oxidation.Water is the ultimate source of electrons in idealized artificial photosynthetic schemes. These electrons may be released during water splitting, preferably utilizing solar energy in aphotoelectrochemical arrangement, and used to produce small molecules such as molecular hydrogen (H 2 ), as olar fuel. Importantly,t his route to H 2 avoids the generation of greenhouse gases. [1] Since the H 2 evolutionr eaction( HER) is much less energy-demanding than the water oxidation reaction (WOR), the later process is considered the limiting step in the overall water splitting scheme,r equiring the use of ac atalyst.M uch effort has been devoted to the development of such catalysts that can perform the WOR for long time periods and at moderate overpotentials.[2] However, little attention has been paid to the influence of the media within which the reaction takes place as aroute to enhance the reactivity of water.The physciochemical properties of water are expected to change in the presence of ions or organic molecules. Such changes can be advantageous as they can be translatedi nto modifications of reactivity.F or instance, Markovice tal. reported that the non-covalent interaction between ions in alkaline solutionsa nd the oxygenated species absorbed on the surface of Ir,R ua nd Ru 0.5 Ir 0.5 electrodes, play an importantr ole in the hydrogene volution reaction (HER), hydrogen oxidation reaction (HOR)a nd oxygen evolution reaction (OER).[3] Particularly, the reactivity towards the HER increasesi nt he order Ba 2 + > Li + > K + .T his trend is explained based on the higher ability of absorbedw ater to be dissociated into H ad and *OH, upon interaction with ions of higher specific charge density.S imilare ffects have been reported by Deng and co-workers,s uggesting that the increased acidity of the water...

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Section: Figuresupporting

confidence: 80%

Section: Figurementioning

confidence: 92%

Section: Figurementioning

confidence: 99%

Section: Figurementioning

confidence: 99%

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Enhanced Reactivity of Water Clusters towards Oxidation in Water/Acetonitrile Mixtures

et al. 2016

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“…Finally, based on our long-term electrolysis and coupled XPS investigations, tuning the affinity of the complex for the polarized electrode surface may be an interesting aspect of catalyst developments, since it has been demonstrated with appropriate polyelectrolyte additives that the layer-by-layer approach is a viable strategy to fabricate OER electrodes. 48,69 …”

Section: Discussionmentioning

confidence: 99%

Armed by Asp? C-terminal carboxylate in a Dap-branched peptide and consequences in the binding of Cu^II and electrocatalytic water oxidation

et al. 2017

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Recent Advances in Electrocatalysis of Oxygen Evolution Reaction using Noble‐Metal, Transition‐Metal, and Carbon‐Based Materials

2020

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A considerable concern in exploring clean, efficient, and renewable energy resources to effectively replace fossil fuels and to combat the environmental problems and energy scarcities for a sustainable future has been observed. In this context, hydrogen is a clean, renewable, energetically efficient fuel with infinite potential for the future, which can generate a large amount of energy through the electrocatalytic splitting of earth‐abundant water resources. Noble metals, owing to their extraordinary efficiency and stability, are state‐of‐the‐art catalysts for the oxygen evolution reaction (OER) process. However, their scarcity and high cost hamper their commercialization. To replace these expensive noble‐metal‐based materials, researchers are extensively working on the development of cost effective, stable, conductive, and efficient non‐noble metal based materials such as transition metal oxides, borides, nitrides, sulfides, phosphides, selenides, perovskites oxides, and layered double hydroxides, where the incorporation of heteroatoms improves the electrocatalytic activity by modifying the electronic structure and enhances the conductivity and stability. In the case of transition‐metal based metal organic frameworks (MOFs) and MOF‐derived materials, the unique structure of MOFs with a high surface area and porosity, as well as rich redox chemistry of transition metals, leads to excellent response towards the OER process. Moreover, direct utilization of carbonaceous materials or making their composites with transition metals not only enhances the conductivity due to their conductive nature but also promotes stability by strongly binding with the electrocatalyst. Owing to the presence of functional groups on the surface or through different interactions, they provide multiple paths for facile electron and ion transport due to the sheet/network like structure, which help in the fine dispersion of electrocatalyst due to high surface area, prevent agglomeration, and in turn results in improved electrocatalytic activity. Besides these advances, a) there is still a need for a thorough understanding of reaction mechanism via in situ spectroscopic techniques to further optimize the composition and design of electrocatalyst to get desired results, b) the stability of the materials should be further enhanced to practically utilize synthesized material under harsh conditions without degradation, and c) the utilization of these optimized OER catalysts in a solar cell to consume solar energy (renewable energy source), remains a key requirement of the modern era.

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Boosting water oxidation layer-by-layer

Cited by 16 publications

References 57 publications

Enhanced Reactivity of Water Clusters towards Oxidation in Water/Acetonitrile Mixtures

Enhanced Reactivity of Water Clusters towards Oxidation in Water/Acetonitrile Mixtures

Armed by Asp? C-terminal carboxylate in a Dap-branched peptide and consequences in the binding of Cu^II and electrocatalytic water oxidation

Recent Advances in Electrocatalysis of Oxygen Evolution Reaction using Noble‐Metal, Transition‐Metal, and Carbon‐Based Materials

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Boosting water oxidation layer-by-layer

Cited by 16 publications

References 57 publications

Enhanced Reactivity of Water Clusters towards Oxidation in Water/Acetonitrile Mixtures

Enhanced Reactivity of Water Clusters towards Oxidation in Water/Acetonitrile Mixtures

Armed by Asp? C-terminal carboxylate in a Dap-branched peptide and consequences in the binding of CuII and electrocatalytic water oxidation

Recent Advances in Electrocatalysis of Oxygen Evolution Reaction using Noble‐Metal, Transition‐Metal, and Carbon‐Based Materials

Contact Info

Product

Resources

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Armed by Asp? C-terminal carboxylate in a Dap-branched peptide and consequences in the binding of Cu^II and electrocatalytic water oxidation