Constructing a Hetero-interface Composed of Oxygen Vacancy-Enriched Co₃O₄ and Crystalline–Amorphous NiFe-LDH for Oxygen Evolution Reaction

ACS Catalysis, Год журнала: 2021, Номер 11(23), С. 14338 - 14351

Опубликована: Ноя. 12, 2021

The development of high-performance electrocatalysts is a highly efficient strategy to optimize the sluggish kinetic property oxygen evolution reaction (OER). Herein, we synthesize kind nickel foam (NF)-supported electrocatalyst composed one-dimensional Co3O4 nanowire as core and two-dimensional NiFe-LDH nanosheet shell (denoted NiFe-60/Co3O4@NF). Fluorine introduced into precursor Co(OH)F Co3O4, which results in improved thermal stability significantly increased regularly distributed vacancies, while electrochemically deposited nanosheets possess crystalline/amorphous hybrid structure. As result, hetero-interface mainly constituting Ni species from contributes interaction between Co Fe facilitates electron transfer. Simultaneously, vacancies coordinatively unsaturated amorphous area also determined, finally completing backtracking. Benefiting these factors, only low overpotentials 221 257 mV are required deliver current densities 100 500 mA cm–2, respectively, with quite small Tafel slope 34.6 dec–1 during OER for well-designed NiFe-60/Co3O4@NF electrocatalyst.

Язык: Английский

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Interfacial electronic modulation by Fe2O3/NiFe-LDHs heterostructures for efficient oxygen evolution at high current density

Applied Catalysis B Environment and Energy, Год журнала: 2022, Номер 306, С. 121097 - 121097

Опубликована: Янв. 13, 2022

Язык: Английский

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Pd–PdO Nanodomains on Amorphous Ru Metallene Oxide for High‐Performance Multifunctional Electrocatalysis

Advanced Materials, Год журнала: 2023, Номер 35(12)

Опубликована: Янв. 4, 2023

Developing highly efficient multifunctional electrocatalysts is crucial for future sustainable energy pursuits, but remains a great challenge. Herein, facile synthetic strategy used to confine atomically thin Pd-PdO nanodomains amorphous Ru metallene oxide (RuO2 ). The as-synthesized electrocatalyst (Pd2 RuOx-0.5 h) exhibits excellent catalytic activity toward the pH-universal hydrogen evolution reaction (η10 = 14 mV in 1 m KOH, η10 12 0.5 H2 SO4 , and 22 PBS), alkaline oxygen 225 mV), overall water splitting (E10 1.49 V) with high mass operational stability. Further reduction endows material RuOx-2 promising activity, evidenced by halfway potential, four-electron selectivity, poison tolerance. enhanced attributed rational integration of favorable nanostructures, including 1) nanosheet morphology, 2) coexisting defective crystalline phases, 3) multi-component heterostructural features. These structural factors effectively regulate material's electronic configuration adsorption intermediates at active sites energetics.

Язык: Английский

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Graphene‐Supported Atomically Dispersed Metals as Bifunctional Catalysts for Next‐Generation Batteries Based on Conversion Reactions

Advanced Materials, Год журнала: 2021, Номер 34(5)

Опубликована: Окт. 22, 2021

Next-generation batteries based on conversion reactions, including aqueous metal-air batteries, nonaqueous alkali metal-O2 and -CO2 metal-chalcogen metal-ion have attracted great interest. However, their use is restricted by inefficient reversible of active agents. Developing bifunctional catalysts to accelerate the reaction kinetics in both discharge charge processes urgently needed. Graphene-, or graphene-like carbon-supported atomically dispersed metal (G-ADMCs) been demonstrated show excellent activity various electrocatalytic making them promising candidates. Different from G-ADMCs for catalysis, which only require high one direction, rechargeable should provide discharging charging. This review provides guidance design fabrication next-generation reactions. The key challenges that prevent conversion, origin G-ADMCs, current principles highly analyzed highlighted each conversion-type battery. Finally, a summary outlook development G-ADMC materials with energy density efficiency are given.

Язык: Английский

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Orbital Occupancy and Spin Polarization: From Mechanistic Study to Rational Design of Transition Metal-Based Electrocatalysts toward Energy Applications

ACS Nano, Год журнала: 2022, Номер 16(11), С. 17847 - 17890

Опубликована: Окт. 31, 2022

Over the past few decades, development of electrocatalysts for energy applications has extensively transitioned from trial-and-error methodologies to more rational and directed designs at atomic levels via either nanogeometric optimization or modulating electronic properties active sites. Regarding modulation properties, nonprecious transition metal-based materials have been attracting large interest due capability versatile tuning d-electron configurations expressed through flexible orbital occupancy various possible degrees spin polarization. Herein, recent advances in tailoring transition-metal atoms intrinsically enhanced electrocatalytic performances are reviewed. We start with discussions on how polarization can govern essential level processes, including transport electron charge bulk, reactive species adsorption catalytic surface, transfer between centers adsorbed as well reaction mechanisms. Subsequently, different techniques currently adopted structures discussed particular emphasis theoretical rationale practical achievements. also highlight promises recently established computational design approaches developing applications. Lastly, discussion is concluded perspectives current challenges future opportunities. hope this review will present beauty structure–activity relationships catalysis sciences contribute advance conversion

Язык: Английский

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Coupling Adsorbed Evolution and Lattice Oxygen Mechanism in Fe‐Co(OH)₂/Fe₂O₃ Heterostructure for Enhanced Electrochemical Water Oxidation

Advanced Functional Materials, Год журнала: 2023, Номер 33(45)

Опубликована: Сен. 1, 2023

Abstract Oxygen evolution reaction (OER) remains a bottleneck for electrocatalytic water‐splitting to generate hydrogen. However, the traditional adsorbed mechanism (AEM) possesses sluggish kinetics due scaling relationship, while lattice oxygen (LOM) triggers an unstable structure escaping of oxygen. Herein, proof‐of‐concept Fe‐Co(OH) 2 /Fe O 3 heterostructure is put forward, where following AEM can complete rapidly deprotonation process Fe LOM trigger O─O coupling step. Combining theoretical and experimental investigation confirmed that redistributed space‐charge junction optimize synergistically oxygen, facilitate synchronously OER activity stability. As result, shows excellent performance with low overpotential only 219 249 mV reach current density 10 100 mA cm −2 . Specifically, electrocatalyst maintains long‐term stability h at large This work paves avenue break through limit conventional mechanism.

Язык: Английский

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Atomically Reconstructed Palladium Metallene by Intercalation-Induced Lattice Expansion and Amorphization for Highly Efficient Electrocatalysis

ACS Nano, Год журнала: 2022, Номер 16(9), С. 13715 - 13727

Опубликована: Авг. 10, 2022

As an emerging class of materials with distinctive physicochemical properties, metallenes are deemed as efficient catalysts for energy-related electrocatalytic reactions. Engineering the lattice strain, electronic structure, crystallinity, and even surface porosity metallene provides a great opportunity to further enhance its catalytic performance. Herein, we rationally developed reconstruction strategy Pd at atomic scale generate series nonmetallic atom-intercalated (M-Pdene, M = H, N, C) expansion S-doped (S-Pdene) amorphous structure. Catalytic performance evaluation demonstrated that N-Pdene exhibited highest mass activities 7.96 A mg-1, which was 10.6 8.5 time greater than those commercial Pd/C Pt/C, respectively, methanol oxidation reaction (MOR). Density functional theory calculations suggested well-controlled tensile strain well strong p-d hybridization interaction between N resulted in enhanced OH adsorption weakened CO MOR catalysis on N-Pdene. When tested hydrogen evolution (HER) catalysts, S-Pdene delivered superior activity durability relative crystalline counterparts because disordered elongated bond length downshifted d-band center. This work effective engineering nanomaterials high electrocatalysts.

Язык: Английский

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Low-Coordination Rhodium Catalysts for an Efficient Electrochemical Nitrate Reduction to Ammonia

ACS Catalysis, Год журнала: 2023, Номер 13(2), С. 1513 - 1521

Опубликована: Янв. 10, 2023

Ammonia is an essential bulk chemical and the main component of fertilizers. In addition, use ammonia (NH3) as energy carrier hydrogen storage material has continuously surged. Electrochemical nitrate reduction a low-carbon, environment-friendly, efficient method synthesis, which attracted extensive attention in recent years; however, overpotential needed to produce NH3 with most catalysts still too large. this work, we rationally designed rhodium nanoflowers (Rh NFs) composed ultrathin nanosheets explored their performance for electrocatalytic (NITRR). With high faradic efficiency 95% at 0.2 V vs reversible electrode (RHE) production, required formation on Rh NF catalyst much lower than previously reported catalysts. X-ray absorption spectroscopy (XAS) analysis shows that there are low-coordination atoms catalyst, can promote adsorption NO3– ions stabilize intermediates revealed by density functional theory (DFT) calculation, resulting NITRR performance.

Язык: Английский

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Recent advances in Ni3S2-based electrocatalysts for oxygen evolution reaction

International Journal of Hydrogen Energy, Год журнала: 2021, Номер 46(79), С. 39146 - 39182

Опубликована: Окт. 19, 2021

Язык: Английский

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Motivating high-valence Nb doping by fast molten salt method for NiFe hydroxides toward efficient oxygen evolution reaction

Chemical Engineering Journal, Год журнала: 2021, Номер 427, С. 131643 - 131643

Опубликована: Авг. 10, 2021

Язык: Английский

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