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A soft molecular 2Fe-2As precursor approach to the synthesis of nanostructured FeAs for efficient electrocatalytic water oxidation.

ABSTRACT: An unprecedented molecular 2Fe-2As precursor complex was synthesized and transformed under soft reaction conditions to produce an active and long-term stable nanocrystalline FeAs material for electrocatalytic water oxidation in alkaline media. The 2Fe2As-centred β-diketiminato complex, having an unusual planar Fe₂As₂ core structure, results from the salt-metathesis reaction of the corresponding β-diketiminato Fe^IICl complex and the AsCO^- (arsaethynolate) anion as the monoanionic As^- source. The as-prepared FeAs phase produced from the precursor has been electrophoretically deposited on conductive electrode substrates and shown to act as a electro(pre)catalyst for the oxygen evolution reaction (OER). The deposited FeAs undergoes corrosion under the severe anodic alkaline conditions which causes extensive dissolution of As into the electrolyte forming finally an active two-line ferrihydrite phase (Fe₂O₃(H₂O) _x ). Importantly, the dissolved As in the electrolyte can be fully recaptured (electro-deposited) at the counter electrode making the complete process eco-conscious. The results represent a new and facile entry to unexplored nanostructured transition-metal arsenides and their utilization for high-performance OER electrocatalysis, which are also known to be magnificent high-temperature superconductors.

SUBMITTER: Beltran-Suito R

PROVIDER: S-EPMC8162750 | biostudies-literature |

REPOSITORIES: biostudies-literature

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A trimetallic organometallic precursor for efficient water oxidation.

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| S-EPMC6403308 | biostudies-literature

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Project description:Water oxidation represents the core process of many sustainable energy systems, such as fuel cells, rechargeable metal-air batteries, and water splitting. Material surface defects with high-energy hanging bonds possess superb intrinsic reactivity, whose actual performance is limited by the dimension and conductivity of the electrocatalyst. Herein we propose a surface defect-rich perovskite electrocatalyst through a p-block metal regulation concept to achieve high performance for oxygen evolution. As a typical p-metal, Sn4+ dissolves from the solid phase from model SnNiFe perovskite nanodots, resulting in abundant surface defects with superior water oxidation performance. An oxygen pool model and a fusion-evolution mechanism are therefore proposed for the in-depth understanding of p-block metal regulation and the oxygen evolution reaction. The energy chemistry unveiled herein provides insights into water oxidation and helps to tackle critical issues in multi-electron oxygen electrocatalysis.Electrocatalysts that possess high densities of surface defects show great promise for efficient water oxidation. Here the authors demonstrate that regulating the p-block metal content in perovskite nanodots imparts these materials with abundant surface defects and excellent electrocatalytic activity.

| S-EPMC5643308 | biostudies-literature

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| S-EPMC10869713 | biostudies-literature

Cobalt Colloid-derived Efficient and Durable Nanoscale Electrocatalytic Films for High-Activity Water Oxidation.

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| S-EPMC7240820 | biostudies-literature

Quasi-single-crystalline CoO hexagrams with abundant defects for highly efficient electrocatalytic water oxidation.

Project description:Defects and structural long-range ordering have been recognized as two crucial characters for advanced electrocatalysts. However, these two features have rarely been achieved together. Herein, we report the preparation of single-crystalline CoO hexagrams and demonstrate their exceptional electrocatalytic properties for water oxidation. The quasi-single-crystalline CoO hexagrams, prepared at the critical phase transition point of ?-Co(OH)2/Co(OH)F hexagrams, possess both abundant oxygen vacancies as defects and structural long-range ordering. The matching between the b-axis of Co(OH)F crystals and the a-axis of ?-Co(OH)2 crystals is critical for the formation of the CoO hexagram single crystals. The quasi-single-crystalline CoO hexagrams with abundant defects are highly efficient for water oxidation by delivering a 10 mA cm-2 current density at a low overpotential of 269 mV in a 1 M KOH aqueous solution.

| S-EPMC6124914 | biostudies-literature

Dendritic core-shell nickel-iron-copper metal/metal oxide electrode for efficient electrocatalytic water oxidation.

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| S-EPMC5786058 | biostudies-literature

Subtle tuning of nanodefects actuates highly efficient electrocatalytic oxidation.

Project description:Achieving controllable fine-tuning of defects in catalysts at the atomic level has become a zealous pursuit in catalysis-related fields. However, the generation of defects is quite random, and their flexible manipulation lacks theoretical basis. Herein, we present a facile and highly controllable thermal tuning strategy that enables fine control of nanodefects via subtle manipulation of atomic/lattice arrangements in electrocatalysts. Such thermal tuning endows common carbon materials with record high efficiency in electrocatalytic degradation of pollutants. Systematic characterization and calculations demonstrate that an optimal thermal tuning can bring about enhanced electrocatalytic efficiency by manipulating the N-centered annulation-volatilization reactions and C-based sp3/sp2 configuration alteration. Benefiting from this tuning strategy, the optimized electrocatalytic anodic membrane successfully achieves >99% pollutant (propranolol) degradation during a flow-through (~2.5 s for contact time), high-flux (424.5 L m-2 h-1), and long-term (>720 min) electrocatalytic filtration test at a very low energy consumption (0.029 ± 0.010 kWh m-3 order-1). Our findings highlight a controllable preparation approach of catalysts while also elucidating the molecular level mechanisms involved.

| S-EPMC10097648 | biostudies-literature

Boosting Water Oxidation through In Situ Electroconversion of Manganese Gallide: An Intermetallic Precursor Approach.

Project description:For the first time, the manganese gallide (MnGa4 ) served as an intermetallic precursor, which upon in situ electroconversion in alkaline media produced high-performance and long-term-stable MnOx -based electrocatalysts for water oxidation. Unexpectedly, its electrocorrosion (with the concomitant loss of Ga) leads simultaneously to three crystalline types of MnOx minerals with distinct structures and induced defects: birnessite ?-MnO2 , feitknechtite ?-MnOOH, and hausmannite ?-Mn3 O4 . The abundance and intrinsic stabilization of MnIII /MnIV active sites in the three MnOx phases explains the superior efficiency and durability of the system for electrocatalytic water oxidation. After electrophoretic deposition of the MnGa4 precursor on conductive nickel foam (NF), a low overpotential of 291?mV, comparable to that of precious-metal-based catalysts, could be achieved at a current density of 10?mA?cm-2 with a durability of more than five days.

| S-EPMC6899514 | biostudies-literature

A Low-Temperature Molecular Precursor Approach to Copper-Based Nano-Sized Digenite Mineral for Efficient Electrocatalytic Oxygen Evolution Reaction.

Project description:In the urge of designing noble metal-free and sustainable electrocatalysts for oxygen evolution reaction (OER), herein, a mineral Digenite Cu9 S5 has been prepared from a molecular copper(I) precursor, [{(PyHS)2 CuI (PyHS)}2 ](OTf)2 (1), and utilized as an anode material in electrocatalytic OER for the first time. A hot injection of 1 yielded a pure phase and highly crystalline Cu9 S5 , which was then electrophoretically deposited (EPD) on a highly conducting nickel foam (NF) substrate. When assessed as an electrode for OER, the Cu9 S5 /NF displayed an overpotential of merely 298±3 mV at a current density of 10 mA cm-2 in alkaline media. The overpotential recorded here supersedes the value obtained for the best reported Cu-based as well as the benchmark precious-metal-based RuO2 and IrO2 electrocatalysts. In addition, the choronoamperometric OER indicated the superior stability of Cu9 S5 /NF, rendering its suitability as the sustainable anode material for practical feasibility. The excellent catalytic activity of Cu9 S5 can be attributed to the formation of a crystalline CuO overlayer on the conductive Cu9 S5 that behaves as active species to facilitate OER. This study delivers a distinct molecular precursor approach to produce highly active copper-based catalysts that could be used as an efficient and durable OER electro(pre)catalysts relying on non-precious metals.

| S-EPMC7155036 | biostudies-literature

Surface Electron-Hole Rich Species Active in the Electrocatalytic Water Oxidation.

Project description:Iridium and ruthenium and their oxides/hydroxides are the best candidates for the oxygen evolution reaction under harsh acidic conditions owing to the low overpotentials observed for Ru- and Ir-based anodes and the high corrosion resistance of Ir-oxides. Herein, by means of cutting edge operando surface and bulk sensitive X-ray spectroscopy techniques, specifically designed electrode nanofabrication and ab initio DFT calculations, we were able to reveal the electronic structure of the active IrOx centers (i.e., oxidation state) during electrocatalytic oxidation of water in the surface and bulk of high-performance Ir-based catalysts. We found the oxygen evolution reaction is controlled by the formation of empty Ir 5d states in the surface ascribed to the formation of formally IrV species leading to the appearance of electron-deficient oxygen species bound to single iridium atoms (μ1-O and μ1-OH) that are responsible for water activation and oxidation. Oxygen bound to three iridium centers (μ3-O) remains the dominant species in the bulk but do not participate directly in the electrocatalytic reaction, suggesting bulk oxidation is limited. In addition a high coverage of a μ1-OO (peroxo) species during the OER is excluded. Moreover, we provide the first photoelectron spectroscopic evidence in bulk electrolyte that the higher surface-to-bulk ratio in thinner electrodes enhances the material usage involving the precipitation of a significant part of the electrode surface and near-surface active species.

| S-EPMC8397309 | biostudies-literature

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