Atomic Cation‐Vacancy Engineering of NiFe‐Layered Double Hydroxides for Improved Activity and Stability towards the Oxygen Evolution Reaction

Angewandte Chemie International Edition, Год журнала: 2021, Номер 60(46), С. 24612 - 24619

Опубликована: Сен. 15, 2021

NiFe-layered double hydroxides (NiFe-LDH) are among the most active catalysts developed to date for oxygen evolution reaction (OER) in alkaline media, though their long-term OER stability remains unsatisfactory. Herein, we reveal that degradation of NiFe-LDH during results from a decreased number sites and undesirable phase segregation form NiOOH FeOOH, with metal dissolution underpinning both these deactivation mechanisms. Further, demonstrate introduction cation-vacancies basal plane NiFe LDH is an effective approach achieving high catalyst activity OER. The strengthened binding energy between metals sheets, together reduced lattice distortions, realized by rational cation vacancies, drastically mitigate under oxidation potentials, resulting improved stability. In addition, vacancies (especially M3+ vacancies) accelerate surface γ-(NiFe)OOH phases, thereby boosting activity. present study highlights tailoring atomic important strategy development stable electrocatalysts.

Язык: Английский

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Hydrogen production coupled with water and organic oxidation based on layered double hydroxides

Exploration, Год журнала: 2021, Номер 1(3)

Опубликована: Дек. 1, 2021

Hydrogen production via electrochemical water splitting is one of the most green and promising ways to produce clean energy address resource crisis, but still suffers from low efficiency high cost mainly due sluggish oxygen evolution reaction (OER) process. Alternatively, hydrogen-evolution coupled with alternative oxidation (EHCO) has been proposed as a considerable strategy improve hydrogen combined value-added chemicals. Although these merits, high-efficient electrocatalysts are always needed in practical operation. Typically, layered double hydroxides (LDHs) have developed large class advanced toward both OER EHCO stability. In this review, we summarized latest progress perspectives designing efficient LDHs-based for EHCO. Particularly, influence structure design component regulation on their electrocatalytic process discussed detail. Finally, look forward challenges field organic oxidation, such mechanism, selected well system design, hoping provide certain inspiration development low-cost technology.

Язык: Английский

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Strategies for designing more efficient electrocatalysts towards the urea oxidation reaction

Journal of Materials Chemistry A, Год журнала: 2022, Номер 10(7), С. 3296 - 3313

Опубликована: Янв. 1, 2022

In this perspective, five typical strategies are summarized for designing highly active electrocatalysts towards the urea oxidation reaction (UOR).

Язык: Английский

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Shining Light on Anion-Mixed Nanocatalysts for Efficient Water Electrolysis: Fundamentals, Progress, and Perspectives

Nano-Micro Letters, Год журнала: 2022, Номер 14(1)

Опубликована: Янв. 3, 2022

Highlights This review introduces recent advances of various anion-mixed transition metal compounds (e.g., nitrides, halides, phosphides, chalcogenides, (oxy)hydroxides, and borides) for efficient water electrolysis applications in detail. The challenges future perspectives are proposed analyzed the dissociation catalysts, including polyanion-mixed metal-free catalyst, progressive synthesis strategies, advanced situ characterizations, atomic level structure–activity relationship. Abstract Hydrogen with high energy density zero carbon emission is widely acknowledged as most promising candidate toward world's neutrality sustainable eco-society. Water-splitting a constructive technology unpolluted high-purity H 2 production, series non-precious electrocatalysts have been developed over past decade. To further improve catalytic activities, doping always adopted to modulate 3 d -electronic configuration electron-donating/accepting (e-DA) properties, while anion doping, electronegativity variations among different non-metal elements would also bring some potential modulations e-DA valence tuning performances. In this review, we summarize developments many (e.g. , oxyhydroxides, borides/borates) applications. First, introduced general information water-splitting description highlighted their complementary functions mixed anions. Furthermore, latest categorized hydrogen oxygen evolution electrocatalysis. rationales behind enhanced electrochemical performances discussed. Last but not least, briefly catalysts.

Язык: Английский

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Reconstruction of Thiospinel to Active Sites and Spin Channels for Water Oxidation

Advanced Materials, Год журнала: 2022, Номер 35(2)

Опубликована: Окт. 25, 2022

Water electrolysis is a promising technique for carbon neutral hydrogen production. A great challenge remains at developing robust and low-cost anode catalysts. Many pre-catalysts are found to undergo surface reconstruction give high intrinsic activity in the oxygen evolution reaction (OER). The reconstructed oxyhydroxides on active species most of them outperform directly synthesized oxyhydroxides. reason be explored. Here, study reported showcase unique behaviors pre-catalyst, thiospinel CoFe2 S4 , its chemistry OER activity. gives mixture with both Fe-S component oxyhydroxide (Co(Fe)Ox Hy ) because Co more inclined reconstruct as oxyhydroxide, while Fe stable major form Fe3 . interface spin channel demonstrated which optimizes energetics steps Co(Fe)Ox facilitates sensitive electron transfer reduce kinetic barrier O-O coupling. advantage also membrane electrode assembly (MEA) electrolyzer. This work introduces feasibility engineering precatalyst performance durable MEA electrolyzers.

Язык: Английский

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Facile growth of hierarchical SnO2@PPy composites on carbon cloth as all-solid-state flexible supercapacitors

Journal of Alloys and Compounds, Год журнала: 2022, Номер 906, С. 164275 - 164275

Опубликована: Фев. 22, 2022

Язык: Английский

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Roles of heteroatoms in electrocatalysts for alkaline water splitting: A review focusing on the reaction mechanism

CHINESE JOURNAL OF CATALYSIS (CHINESE VERSION), Год журнала: 2022, Номер 43(8), С. 2091 - 2110

Опубликована: Июнь 24, 2022

Язык: Английский

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Introducing High‐Valence Iridium Single Atoms into Bimetal Phosphides toward High‐Efficiency Oxygen Evolution and Overall Water Splitting

Small, Год журнала: 2023, Номер 19(15)

Опубликована: Янв. 6, 2023

Single atoms are superior electrocatalysts having high atomic utilization and amazing activity for water oxidation splitting. Herein, this work reports a thermal reduction method to introduce high-valence iridium (Ir) single into bimetal phosphide (FeNiP) nanoparticles toward high-efficiency oxygen evolution reaction (OER) overall The presence of Ir (Ir4+ ) their synergistic interaction with Ni3+ species as well the disproportionation assisted by Fe collectively contribute exceptional OER performance. In specific, at appropriate Ir/Ni Fe/Ni ratios, as-prepared Ir-doped FeNiP (Ir25 -Fe16 Ni100 P64 mass loading only 35 µg cm-2 show overpotential low 232 mV 10 mA 1.86 A mg-1 1.5 V versus RHE in 1.0 m KOH. Computational simulations confirm vital role weaken adsorption intermediates, favorable accelerating kinetics. Impressively, Pt/C||Ir25 two-electrode alkaline electrolyzer affords current density cell voltage 1.42 V, along satisfied stability. An AA battery nominal can drive splitting obvious bubbles released.

Язык: Английский

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Hierarchical Crystalline/Amorphous Heterostructure MoNi/NiMoO_x for Electrochemical Hydrogen Evolution with Industry‐Level Activity and Stability

Advanced Functional Materials, Год журнала: 2023, Номер 33(41)

Опубликована: Авг. 27, 2023

Abstract The design of cheap, efficient, and durable electrocatalysts for high‐throughput H 2 production is critical to give impetus hydrogen from fundamental practical industrial applications. Here, a hierarchical heterostructure evolution reaction (HER) electrocatalyst (MoNi/NiMoO x ) with 0D MoNi nanoalloys nanoparticles embedded on well‐assembled 1D porous NiMoO microrods in situ grown 3D nickel foam (NF) successfully constructed. synergetic effect different building units the unique structure endows MoNi/NiMoO composites highly active heterogeneous interface low water dissociation energy (Δ G diss = −1.2 eV) optimized adsorption ability H* −0.01 eV), fast electron/mass transport, strong catalyst‐support binding force. As result, optimal exhibits an ampere‐level current density 1.9 A cm −2 at ultralow overpotential 139 mV 1.0 м KOH 289 PBS solution, respectively. Particularly, scaled‐up electrodes 10 × membrane electrode assembly (MEA) electrolyzer reach high rate 12.12 L h −1 (12.12 times than that commercial NF) exhibit ultralong stability 1600 h, verifying its huge potential production.

Язык: Английский

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Exploring Ir-doped NiFe-LDH nanosheets via a pulsed laser for oxygen evolution kinetics: in situ Raman and DFT insights

Journal of Materials Chemistry A, Год журнала: 2024, Номер 12(15), С. 8694 - 8706

Опубликована: Янв. 1, 2024

Herein, we present Ir-doped NiFe-LDH nanosheets synthesized via a pulsed laser irradiation strategy, showing superior electrocatalytic OER kinetics. We investigate the origin of activity in NiFeIr-LDH through situ / operando Raman and DFT studies.

Язык: Английский

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