A surface-modified antiperovskite as an electrocatalyst for water oxidation.
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ABSTRACT:
SUBMITTER: Zhu Y
PROVIDER: S-EPMC5997991 | biostudies-literature |
REPOSITORIES: biostudies-literature
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Project description:High-entropy materials are an emerging pathway in the development of high-activity (electro)catalysts because of the inherent tunability and coexistence of multiple potential active sites, which may lead to earth-abundant catalyst materials for energy-efficient electrochemical energy storage. In this report, we identify how the multication composition in high-entropy perovskite oxides (HEO) contributes to high catalytic activity for the oxygen evolution reaction (OER), i.e., the key kinetically limiting half-reaction in several electrochemical energy conversion technologies, including green hydrogen generation. We compare the activity of the (001) facet of LaCr0.2Mn0.2Fe0.2Co0.2Ni0.2O3-δ with the parent compounds (single B-site in the ABO3 perovskite). While the single B-site perovskites roughly follow the expected volcano-type activity trends, the HEO clearly outperforms all of its parent compounds with 17 to 680 times higher currents at a fixed overpotential. As all samples were grown as an epitaxial layer, our results indicate an intrinsic composition-function relationship, avoiding the effects of complex geometries or unknown surface composition. In-depth X-ray photoemission studies reveal a synergistic effect of simultaneous oxidation and reduction of different transition metal cations during the adsorption of reaction intermediates. The surprisingly high OER activity demonstrates that HEOs are a highly attractive, earth-abundant material class for high-activity OER electrocatalysts, possibly allowing the activity to be fine-tuned beyond the scaling limits of mono- or bimetallic oxides.
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Project description:The development of highly efficient electrocatalysts toward the oxygen evolution reaction is imperative for advancing water splitting technology to generate clean hydrogen energy. Herein, a two dimensional (2D) nanosheet ammonium cobalt phosphate hydrate (NH4CoPO4·H2O) catalyst based on the earth-abundant non-noble metal is reported. When used for the challenging alkaline saline water electrolysis, the NH4CoPO4·H2O catalyst with the optimal thickness of 30 nm achieves current densities of 10 and 100 mA cm-2 at the record low overpotentials of 252 and 268 mV, respectively, while maintaining remarkable stability during the alkaline saline water oxidation at room temperature. X-ray absorption fine spectra reveal that the activation of Co (II) ions (in NH4CoPO4·H2O) to Co (III) species constructs the electrocatalytic active sites. The 2D nanosheet morphology of NH4CoPO4·H2O provides a larger active surface area and more surface-exposed active sites, which enable the nanosheet catalyst to facilitate the alkaline freshwater and simulated seawater oxidation with excellent activity. The facile and environmentally-benign H2O-mediated synthesis route under mild condition makes NH4CoPO4·H2O catalyst highly feasible for practical manufacturing. In comparison with noble metals, this novel electrocatalyst offers a cost-effective alternative for economic saline water oxidation to advance water electrolysis technology.
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Project description:Layered double hydroxides (LDH) are being used as electrocatalysts for oxygen evolution reactions (OERs). However, low current densities limit their practical applications. Herein, we report a facile and economic synthesis of an iron-copper based LDH integrated with a cobalt-based metal-organic framework (ZIF-12) to form LDH-ZIF-12 composite (1) through a co-precipitation method. The as-synthesized composite 1 requires a low overpotential of 337 mV to achieve a catalytic current density of 10 mA cm-2 with a Tafel slope of 89 mV dec-1. Tafel analysis further demonstrates that 1 exhibits a slope of 89 mV dec-1 which is much lower than the slope of 284 mV dec-1 for LDH and 172 mV dec-1 for ZIF-12. The slope value of 1 is also lower than previously reported electrocatalysts, including Ni-Co LDH (113 mV dec-1) and Zn-Co LDH nanosheets (101 mV dec-1), under similar conditions. Controlled potential electrolysis and stability test experiments show the potential application of 1 as a heterogeneous electrocatalyst for water oxidation.
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Project description:Developing a cost-effective, efficient, and stable oxygen evolution reaction (OER) catalyst is of great importance for sustainable energy conversion and storage. In this study, we report a facile one-step fabrication of cationic surfactant-assisted Prussian blue analogues (PBAs) Mx[Fe(CN)5CH3C6H4NH2]∙yC19H34NBr abbreviated as SF[Fe-Tol-M] (where SF = N-tridecyl-3-methylpyridinium bromide and M = Mn, Co and Ni) as efficient heterogeneous OER electrocatalysts. The electrocatalysts have been characterized by Fourier transform infrared (FT-IR) spectroscopy, powder X-ray diffraction (PXRD), scanning electron microscopy (SEM) coupled with energy dispersive X-ray (EDX) analysis, and X-ray photoelectron spectroscopy (XPS). In the presence of cationic surfactant (SF), PBAs-based electrodes showed enhanced redox current, high surface area and robust stability compared to the recently reported PBAs. SF[Fe-Tol-Co] hybrid catalyst shows superior electrochemical OER activity with a much lower over-potential (610 mV) to attain the current density of 10 mA cm-2 with the Tafel slope value of 103 mV·dec-1 than that for SF[Fe-Tol-Ni] and SF[Fe-Tol-Mn]. Moreover, the electrochemical impedance spectroscopy (EIS) unveiled that SF[Fe-Tol-Co] exhibits smaller charge transfer resistance, which results in a faster kinetics towards OER. Furthermore, SF[Fe-Tol-Co] offered excellent stability for continues oxygen production over extended reaction time. This work provides a surface assisted facile electrode fabrication approach for developing binder-free OER electrocatalysts for efficient water oxidation.
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Project description:Active and highly stable electrocatalysts for oxygen evolution reaction (OER) in acidic media are currently in high demand as a cleaner alternative to the combustion of fossil fuels. Herein, we report a Co-doped nanorod-like RuO2 electrocatalyst with an abundance of oxygen vacancies achieved through the facile, one-step annealing of a Ru-exchanged ZIF-67 derivative. The compound exhibits ultra-high OER performance in acidic media, with a low overpotential of 169 mV at 10 mA cm-2 while maintaining excellent activity, even when exposed to a 50-h galvanostatic stability test at a constant current of 10 mA cm-2. The dramatic enhancement in OER performance is mainly attributed to the abundance of oxygen vacancies and modulated electronic structure of the Co-doped RuO2 that rely on a vacancy-related lattice oxygen oxidation mechanism (LOM) rather than adsorbate evolution reaction mechanism (AEM), as revealed and supported by experimental characterizations as well as density functional theory (DFT) calculations.
| S-EPMC6941840 | biostudies-literature
Project description:The design and fabrication of intricate hollow architectures as cost-effective and dual-function electrocatalyst for water and urea electrolysis is of vital importance to the energy and environment issues. Herein, a facile solvothermal strategy for construction of Prussian-blue analogue (PBA) hollow cages with an open framework was developed. The as-obtained CoFe and NiFe hollow cages (CFHC and NFHC) can be directly utilized as electrocatalysts towards oxygen evolution reaction (OER) and urea oxidation reaction (UOR) with superior catalytic performance (lower electrolysis potential, faster reaction kinetics and long-term durability) compared to their parent solid precursors (CFC and NFC) and even the commercial noble metal-based catalyst. Impressively, to drive a current density of 10?mA?cm-2 in alkaline solution, the CFHC catalyst required an overpotential of merely 330?mV, 21.99% lower than that of the solid CFC precursor (423?mV) at the same condition. Meanwhile, the NFHC catalyst could deliver a current density as high as 100?mA?cm-2 for the urea oxidation electrolysis at a potential of only 1.40?V, 24.32% lower than that of the solid NFC precursor (1.85?V). This work provides a new platform to construct intricate hollow structures as promising nano-materials for the application in energy conversion and storage.
| S-EPMC6828720 | biostudies-literature
Project description:Production of hydrogen through water splitting is one of the green and the most practical solutions to cope with the energy crisis and greenhouse effect. However, oxygen evolution reaction (OER) being a sluggish step, the use of precious metal-based catalysts is the main impediment toward the viability of water splitting. In this work, amorphous copper oxide and doped binary- and ternary-metal oxides (containing CoII, NiII, and CuII) have been prepared on the surface of fluorine-doped tin oxide by a facile electrodeposition route followed by thermal treatment. The fabricated electrodes have been employed as efficient binder-free OER electrocatalysts possessing a high electrochemical surface area due to their amorphous nature. The cobalt-nickel-doped copper oxide (ternary-metal oxide)-based electrode showed promising OER activity with a high current density of 100 mA cm-2 at 1.65 V versus RHE that escalates to 313 mA cm-2 at 1.76 V in alkaline media at pH 14. The high activity of the ternary-metal oxide-based electrode was further supported by a smaller semicircle in the Nyquist plot. Furthermore, all metal-oxide-based electrodes offered high stability when tested for continuous production of oxygen for 50 h. This work highlights the synthesis of efficient and cost-effective amorphous metal-based oxide catalysts to execute electrocatalytic OER employing an electrodeposition approach.
| S-EPMC8340103 | biostudies-literature
Project description:We investigate LaCo2P2 as an electrocatalytic material for oxygen evolution reaction (OER) under alkaline and acidic conditions. This layered intermetallic material was prepared via Sn-flux high-temperature annealing. The electrocatalytic ink, prepared with the ball-milled LaCo2P2 catalyst at the mass loading of 0.25 mg/cm2, shows OER activity at pH = 14, reaching current densities of 10, 50, and 100 mA/cm2 under the overpotential of 400, 440, and 460 mV, respectively. Remarkably, the electrocatalytic performance remains constant for at least 4 days. Transmission electron microscopy reveals the formation of a catalytically active CoOx shell around the pre-catalyst LaCo2P2 core during the alkaline OER. The core serves as a robust support for the in situ-formed electrocatalytic system. Similar studies under pH = 0 reveal the rapid deterioration of LaCo2P2, with the formation of LaPO4 and amorphous cobalt oxide. This study shows the viability of layered intermetallics as stable OER electrocatalysts, although further developments are required to improve the electrocatalytic performance and increase the stability at lower pH values.
| S-EPMC9455929 | biostudies-literature
Project description:Three dimensional (3D) porous carbon materials are highly desirable for electrochemical applications owing to their high surface area and porosity. Uniformly distributed porosity in the 3D architecture of carbon support materials allows reactant molecules to access more electrochemically active centres and simultaneously facilitate removal of the product formed during electrochemical reactions. Herein, we have prepared a nitrogen-doped entangled graphene framework (NEGF), decorated with NiFe-LDH nanostructures by an in situ solvothermal method followed by freeze-drying at high vacuum pressure and low temperature. The freeze-drying method helped to prevent the restacking of the graphene sheets and the formation of a high surface area nitrogen-doped entangled graphene framework (NEGF) supported NiFe-LDHs. The incorporation of the NEGF has significantly reduced the overpotential for the electrochemical oxygen evolution reaction (OER) in 1 M KOH solution. This corresponds to an overpotential reduction from 340 mV for NiFe-LDHs to 290 mV for NiFe-LDH/NEGF to reach the benchmark current density of 10 mA cm-2. The preparation of the catalyst is conceived through a low-temperature scalable process.
| S-EPMC9419039 | biostudies-literature
Project description:The design of oxygen evolution reaction (OER) catalysts with higher stability and activity by economical and convenient methods is considered particularly important for the energy conversion technology. Herein, a simple hydrothermal method was adopted for the synthesis of iodine-doped nickel hydroxide nanoparticles and their OER performance was explored. The electrocatalysts were structurally characterized by powder X-ray diffraction analysis (P-XRD), Fourier transform infrared spectroscopy (FTIR), field emission scanning electron microscopy (FESEM), energy dispersive X-ray spectroscopy (EDX), and BET analysis. The electrochemical performance of the electrocatalysts was assessed by cyclic voltammetry, linear sweep voltammetry, and electrochemical impedance spectroscopy. The abundant catalytic active sites, oxygen vacancies, low charge-transfer resistance, and a high pore diameter to pore size ratio of iodine-doped Ni(OH)2 were responsible for its excellent catalytic activity, whereby OER was initiated even at 1.52 V (vs. RHE) and a 330 mV overpotential was needed to reach a 40 mV cm-2 current density in 1 M KOH solution. The material also exhibited a low Tafel slope (46 mV dec-1), which suggests faster charge-transfer kinetics as compared to its counterparts tested under the same electrochemical environment. It is worth noting that this facile and effective approach suggests a new way for the fabrication of metal hydroxides rich in oxygen vacancies, thus with the potential to boost the electrochemical performance of energy-related systems.
| S-EPMC9386693 | biostudies-literature