Synergistic effect of multiple vacancies to induce lattice oxygen redox in NiFe-layered double hydroxide OER catalysts

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 323, P. 122091 - 122091

Published: Nov. 3, 2022

Language: Английский

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Designing a Built-In Electric Field for Efficient Energy Electrocatalysis

ACS Nano, Journal Year: 2022, Volume and Issue: 16(12), P. 19959 - 19979

Published: Dec. 15, 2022

To utilize intermittent renewable energy as well achieve the goals of peak carbon dioxide emissions and neutrality, various electrocatalytic devices have been developed. However, reactions, e.g., hydrogen evolution reaction/oxygen reaction in overall water splitting, polysulfide conversion lithium–sulfur batteries, formation/decomposition lithium peroxide lithium–oxygen nitrate reduction to degrade sewage, suffer from sluggish kinetics caused by multielectron transfer processes. Owing merits accelerated charge transport, optimized adsorption/desorption intermediates, raised conductivity, regulation microenvironment, ease combine with geometric characteristics, built-in electric field (BIEF) is expected overcome above problems. Here, we give a Review about very recent progress BIEF for efficient electrocatalysis. First, construction strategies characterization methods (qualitative quantitative analysis) are summarized. Then, up-to-date overviews engineering electrocatalysis, attention on electron structure optimization microenvironment modulation, analyzed discussed detail. In end, challenges perspectives proposed. This gives deep understanding design electrocatalysts next-generation storage devices.

Language: Английский

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Hydroxyl-Bonded Ru on Metallic TiN Surface Catalyzing CO₂ Reduction with H₂O by Infrared Light

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(50), P. 27415 - 27423

Published: Dec. 11, 2023

Synchronized conversion of CO2 and H2O into hydrocarbons oxygen via infrared-ignited photocatalysis remains a challenge. Herein, the hydroxyl-coordinated single-site Ru is anchored precisely on metallic TiN surface by NaBH4/NaOH reforming method to construct an infrared-responsive HO-Ru/TiN photocatalyst. Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (ac-HAADF-STEM) X-ray absorption spectroscopy (XAS) confirm atomic distribution species. XAS density functional theory (DFT) calculations unveil formation HO-RuN5-Ti Lewis pair sites, which achieves efficient polarization/activation dual coordination with C O atoms HO-Ru/TiN. Also, implanting species powerfully boosts separation transfer photoinduced charges. Under infrared irradiation, catalyst shows superior CO2-to-CO transformation activity coupled oxidation release O2, reduction rate can further be promoted about 3-fold under simulated sunlight. With key reaction intermediates determined in situ diffuse reflectance Fourier transform (DRIFTS) predicted DFT simulations, possible photoredox mechanism system proposed.

Language: Английский

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Amorphous/Crystalline Heterostructure Transition-Metal-based Catalysts for High-Performance Water Splitting

Coordination Chemistry Reviews, Journal Year: 2022, Volume and Issue: 475, P. 214916 - 214916

Published: Oct. 31, 2022

Language: Английский

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Recent Advances in Carbon‐Supported Noble‐Metal Electrocatalysts for Hydrogen Evolution Reaction: Syntheses, Structures, and Properties

Advanced Energy Materials, Journal Year: 2022, Volume and Issue: 12(28)

Published: June 2, 2022

Abstract The electrochemical hydrogen evolution reaction (HER) that converts renewable electricity into storable hydrogen, a sustainable and clean energy carrier, provides promising method to mitigate the crisis environmental pollution. In general, noble‐metal‐based nanomaterials (including Pt, Rh, Ru, Ir, etc.) have drawn tremendous research attention in context of HER because their nearly optimal bindings robust stability tunable physical/chemical properties. Particularly, carbon as substrate not only offers stabilizing conductive matrix, but also impacts electronic structure supported metal by interfacial interaction, necessitating detailed understanding. To speed up sluggish kinetics HER, design construction efficient electrocatalysts is crucial importance. Herein, comprehensive review recent advances carbon‐supported noble‐metal presented, focusing on synthetic strategies, structural analyses, applications electrocatalysis. Specifically, correlation between activity discussed. Furthermore, perspective offered highlighting challenges opportunities for development highly electrocatalysts, with aim widespread utilization practical water electrolyzers toward green production.

Language: Английский

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Self‐Reconstructed Metal‐Organic Framework Heterojunction for Switchable Oxygen Evolution Reaction

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(51)

Published: Oct. 24, 2022

Designing metal-organic framework (MOF)-based catalysts with superior oxygen evolution reaction (OER) activity and robust durability simultaneously is highly required yet very challenging due to the limited intrinsic their elusive under harsh OER conditions. Herein, a steady self-reconstructed MOF heterojunction constructed via redox electrochemistry topology-guided strategy. Thanks inhibiting effect from hydrogen bonds of Ni-BDC-1 (BDC=1,4-benzenedicarboxylic acid), obatained shows greatly improved low overpotential 225 mV at 10 mA cm-2 , relative totally reconstructed Ni-BDC-3 (332 mV). Density function theory calculations reveal that formed built-in electric field in remarkably optimizes ad/desorption free energy active Ni sites. Moreover, such attributed shielding surface-evolved NiOOH coating.

Language: Английский

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Ir Nanoparticles Anchored on Metal‐Organic Frameworks for Efficient Overall Water Splitting under pH‐Universal Conditions

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(17)

Published: March 2, 2023

The construction of high-activity and low-cost electrocatalysts is critical for efficient hydrogen production by water electrolysis. Herein, we developed an advanced electrocatalyst anchoring well-dispersed Ir nanoparticles on nickel metal-organic framework (MOF) Ni-NDC (NDC: 2,6-naphthalenedicarboxylic) nanosheets. Benefiting from the strong synergy between MOF through interfacial Ni-O-Ir bonds, synthesized Ir@Ni-NDC showed exceptional electrocatalytic performance evolution reaction (HER), oxygen (OER) overall splitting in a wide pH range, superior to commercial benchmarks most reported electrocatalysts. Theoretical calculations revealed that charge redistribution bridge induced optimization H2 O, OH* H* adsorption, thus leading accelerated electrochemical kinetics HER OER. This work provides new clue exploit bifunctional pH-universal splitting.

Language: Английский

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Collaborative Interface Optimization Strategy Guided Ultrafine RuCo and MXene Heterostructure Electrocatalysts for Efficient Overall Water Splitting

ACS Nano, Journal Year: 2023, Volume and Issue: 17(11), P. 10947 - 10957

Published: May 18, 2023

Developing highly active and robust electrocatalysts for the hydrogen/oxygen evolution reaction (HER/OER) is crucial large-scale utilization of green hydrogen. In this study, a collaborative interface optimization guided strategy was employed to prepare metal-organic framework (MOF) derived heterostructure electrocatalyst (MXene@RuCo NPs). The obtained requires overpotentials only 20 mV HER 253 OER deliver current density 10 mA/cm2 in alkaline media, respectively, it also exhibits great performance at high density. Experiments theoretical calculations reveal that doped Ru introduces second sites decreases diameter nanoparticles, which greatly enhances number sites. More importantly, MXene/RuCo NPs heterogeneous interfaces catalysts exhibit synergistic effects, decreasing work function catalyst improving charge transfer rate, thus reducing energy barrier catalytic reaction. This represents promising development MOF-derived achieve efficient conversion industrial applications.

Language: Английский

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Design of modified MOFs electrocatalysts for water splitting: High current density operation and long-term stability

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 336, P. 122891 - 122891

Published: May 18, 2023

Language: Английский

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Electronic Modulation of Metal–Organic Frameworks by Interfacial Bridging for Efficient pH‐Universal Hydrogen Evolution

Advanced Functional Materials, Journal Year: 2022, Volume and Issue: 33(1)

Published: Oct. 26, 2022

Abstract Designing well‐defined interfacial chemical bond bridges is an effective strategy to optimize the catalytic activity of metal–organic frameworks (MOFs), but it remains challenging. Herein, a facile in situ growth reported for synthesis tightly connected 2D/2D heterostructures by coupling MXene with CoBDC nanosheets. The multifunctional nanosheets high conductivity and ideal hydrophilicity as bridging carriers can ensure structural stability sufficient exposure active sites. Moreover, Co–O–Ti formed at interface effectively triggers charge transfer modulates electronic structure Co‐active site, which enhances reaction kinetics. As result, optimized CoBDC/MXene exhibits superior hydrogen evolution (HER) low overpotentials 29, 41, 76 mV 10 mA cm −2 alkaline, acidic, neutral electrolytes, respectively, comparable commercial Pt/C. Theoretical calculation demonstrates that bridging‐induced electron redistribution optimizes free energy water dissociation adsorption, resulting improved evolution. This study not only provides novel electrocatalyst efficient HER all pH conditions also opens up new avenue designing highly systems.

Language: Английский

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