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An Unconventional Iron Nickel Catalyst for the Oxygen Evolution Reaction.

ABSTRACT: The oxygen evolution reaction (OER) is a key process that enables the storage of renewable energies in the form of chemical fuels. Here, we describe a catalyst that exhibits turnover frequencies higher than state-of-the-art catalysts that operate in alkaline solutions, including the benchmark nickel iron oxide. This new catalyst is easily prepared from readily available and industrially relevant nickel foam, and it is stable for many hours. Operando X-ray absorption spectroscopic data reveal that the catalyst is made of nanoclusters of ?-FeOOH covalently linked to a ?-NiOOH support. According to density functional theory (DFT) computations, this structure may allow a reaction path involving iron as the oxygen evolving center and a nearby terrace O site on the ?-NiOOH support oxide as a hydrogen acceptor.

SUBMITTER: Song F

PROVIDER: S-EPMC6439451 | biostudies-literature | 2019 Mar

REPOSITORIES: biostudies-literature

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An Unconventional Iron Nickel Catalyst for the Oxygen Evolution Reaction.

Song Fang F Busch Michael M MM Lassalle-Kaiser Benedikt B Hsu Chia-Shuo CS Petkucheva Elitsa E Bensimon Michaël M Chen Hao Ming HM Chen Hao Ming HM Corminboeuf Clemence C Hu Xile X

ACS central science 20190226 3

The oxygen evolution reaction (OER) is a key process that enables the storage of renewable energies in the form of chemical fuels. Here, we describe a catalyst that exhibits turnover frequencies higher than state-of-the-art catalysts that operate in alkaline solutions, including the benchmark nickel iron oxide. This new catalyst is easily prepared from readily available and industrially relevant nickel foam, and it is stable for many hours. Operando X-ray absorption spectroscopic data reveal tha ...[more]

PMID: 30937383

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A nickel iron diselenide-derived efficient oxygen-evolution catalyst.

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Project description:The incorporation of defects, such as vacancies, into functional materials could substantially tailor their intrinsic properties. Progress in vacancy chemistry has enabled advances in many technological applications, but creating new type of vacancies in existing material system remains a big challenge. We show here that ionized nitrogen plasma can break bonds of iron-carbon-nitrogen-nickel units in nickel-iron Prussian blue analogues, forming unconventional carbon-nitrogen vacancies. We study oxygen evolution reaction on the carbon-nitrogen vacancy-mediated Prussian blue analogues, which exhibit a low overpotential of 283 millivolts at 10 milliamperes per square centimeter in alkali, far exceeding that of original Prussian blue analogues and previously reported oxygen evolution catalysts with vacancies. We ascribe this enhancement to the in-situ generated nickel-iron oxy(hydroxide) active layer during oxygen evolution reaction, where the Fe leaching was significantly suppressed by the unconventional carbon-nitrogen vacancies. This work opens up opportunities for producing vacancy defects in nanomaterials for broad applications.

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Reaction pathways for oxygen evolution promoted by cobalt catalyst.

Project description:The in-depth understanding of the molecular mechanisms regulating the water oxidation catalysis is of key relevance for the rationalization and the design of efficient oxygen evolution catalysts based on earth-abundant transition metals. Performing ab initio DFT+U molecular dynamics calculations of cluster models in explicit water solution, we provide insight into the pathways for oxygen evolution of a cobalt-based catalyst (CoCat). The fast motion of protons at the CoCat/water interface and the occurrence of cubane-like Co-oxo units at the catalyst boundaries are the keys to unlock the fast formation of O-O bonds. Along the resulting pathways, we identified the formation of Co(IV)-oxyl species as the driving ingredient for the activation of the catalytic mechanism, followed by their geminal coupling with O atoms coordinated by the same Co. Concurrent nucleophilic attack of water molecules coming directly from the water solution is discouraged by high activation barriers. The achieved results suggest also interesting similarities between the CoCat and the Mn4Ca-oxo oxygen evolving complex of photosystem II.

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Nonmetallic Active Sites on Nickel Phosphide in Oxygen Evolution Reaction.

Project description:Efficient and durable catalysts are crucial for the oxygen evolution reaction (OER). The discovery of the high OER catalytic activity in Ni12P5 has attracted a great deal of attention recently. Herein, the microscopic mechanism of OER on the surface of Ni12P5 is studied using density functional theory calculations (DFT) and ab initio molecular dynamics simulation (AIMD). Our results demonstrate that the H2O molecule is preferentially adsorbed on the P atom instead of on the Ni atom, indicating that the nonmetallic P atom is the active site of the OER reaction. AIMD simulations show that the dissociation of H from the H2O molecule takes place in steps; the hydrogen bond changes from Oa-H⋯Ob to Oa⋯H-Ob, then the hydrogen bond breaks and an H+ is dissociated. In the OER reaction on nickel phosphides, the rate-determining step is the formation of the OOH group and the overpotential of Ni12P5 is the lowest, thus showing enhanced catalytic activity over other nickel phosphides. Moreover, we found that the charge of Ni and P sites has a linear relationship with the adsorption energy of OH and O, which can be utilized to optimize the OER catalyst.

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Direct MOCVD Growth of Iron Oxide on Three-Dimensional Nickel Foam as Electrode for the Oxygen Evolution Reaction.

Project description:Iron oxide thin films were grown directly on three-dimensional nickel foam via metalorganic chemical vapor deposition (MOCVD) in the temperature range of 250-450 °C using Fe(CO)5 as precursor. Iron oxide (α-Fe2 O3 ) films were formed at low substrate temperatures (250-350 °C), whereas the additional growth of an underlying NiO film occurred at substrate temperatures above 350 °C. The electrochemical activities of the as-formed binder-free and noble metal-free electrodes were tested for the oxygen evolution reaction (OER) in alkaline media. An overpotential reduced by 250 mV at a current density of 50 mA cm-2 and a lower Tafel slope of 55 mV dec-1 compared to bare nickel foam were found for the best-performing electrocatalyst, while the long-term stability of the as-formed electrodes was proven by chronopotentiometry. The surface morphology of the iron oxide films was characterized by scanning electron microscopy, whereas the crystallographic phase as well as the elemental composition were determined by X-ray diffraction, energy-dispersive X-ray spectroscopy, X-ray photoelectron spectroscopy, and time-of-flight secondary ion mass spectrometry in the pre- and the post-catalytic state.

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Oxygen-evolution reaction by nickel/nickel oxide interface in the presence of ferrate(VI).

Project description:In this study, we investigate the effect of K2FeO4, as a new and soluble Fe salt at alkaline conditions, on oxygen-evolution reaction (OER) of Ni oxide. Both oxidation and reduction peaks for Ni in the presence and absence of Fe are linearly changed by (scan rate)1/2. Immediately after the interaction of [FeO4]2- with the surface of the electrode, a significant increase in OER is observed. This could be indicative of the fact that either the [FeO4]2- on the surface of Ni oxide is directly involved in OER, or, it is important to activate Ni oxide toward OER. Due to the change in the Ni(II)/(III) peak, it is hypothesized that Fe impurity in KOH or electrochemical cell has different effects at the potential range. At low potential, [FeO4]2- is reduced on the surface of the electrode, and thus, is significantly adsorbed on the electrode. Finally, oxygen-evolution measurements of K2FeO4 and Ni2O3 are investigated under chemical conditions. K2FeO4 is not stable in the presence of Ni(II) oxide, and OER is observed in a KOH solution (pH ≈ 13).

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