Facet Engineering of Advanced Electrocatalysts Toward Hydrogen/Oxygen Evolution Reactions

Nano-Micro Letters, Journal Year: 2023, Volume and Issue: 15(1)

Published: Feb. 16, 2023

The electrocatalytic water splitting technology can generate high-purity hydrogen without emitting carbon dioxide, which is in favor of relieving environmental pollution and energy crisis achieving neutrality. Electrocatalysts effectively reduce the reaction barrier increase efficiency. Facet engineering considered as a promising strategy controlling ratio desired crystal planes on surface. Owing to anisotropy, with different orientations usually feature facet-dependent physical chemical properties, leading differences adsorption energies oxygen or intermediates, thus exhibit varied activity toward evolution (HER) (OER). In this review, brief introduction basic concepts, fundamental understanding mechanisms well key evaluating parameters for both HER OER are provided. formation facets comprehensively overviewed aiming give scientific theory guides realize dominant planes. Subsequently, three strategies selective capping agent, etching coordination modulation tune summarized. Then, we present an overview significant contributions facet-engineered catalysts HER, OER, overall splitting. particular, highlight that density functional calculations play indispensable role unveiling structure–activity correlation between plane catalytic activity. Finally, remaining challenges provided future prospects designing advanced electrocatalysts discussed.

Language: 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, Journal Year: 2023, Volume and Issue: 33(45)

Published: Sept. 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.

Language: Английский

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Defect Engineered Metal–Organic Framework with Accelerated Structural Transformation for Efficient Oxygen Evolution Reaction

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(43)

Published: Sept. 6, 2023

Metal-organic frameworks (MOFs) have been increasingly applied in oxygen evolution reaction (OER), and the surface of MOFs usually undergoes structural transformation to form metal oxyhydroxides serve as catalytically active sites. However, controllable regulation reconstruction process remains a great challenge. Here we report defect engineering strategy facilitate during OER with enhanced activity. Defective (denoted NiFc'x Fc1-x ) abundant unsaturated sites are constructed by mixing ligands 1,1'-ferrocene dicarboxylic acid (Fc') defective ferrocene carboxylic (Fc). series more prone be transformed compared non-defective (NiFc'). Moreover, as-formed derived from contain vacancies. NiFc'Fc grown on nickel foam exhibits excellent catalytic activity an overpotential 213 mV at current density 100 mA cm-2 , superior that undefective NiFc'. Experimental results theoretical calculations suggest vacancies adsorption oxygen-containing intermediates centers, thus significantly improving

Language: Английский

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High‐Valence Oxides for High Performance Oxygen Evolution Electrocatalysis

Advanced Science, Journal Year: 2023, Volume and Issue: 10(22)

Published: May 30, 2023

Valence tuning of transition metal oxides is an effective approach to design high-performance catalysts, particularly for the oxygen evolution reaction (OER) that underpins solar/electric water splitting and metal-air batteries. Recently, high-valence (HVOs) are reported show superior OER performance, in association with fundamental dynamics charge transfer intermediates. Particularly considered adsorbate mechanism (AEM) lattice oxygen-mediated (LOM). High-valence states enhance performance mainly by optimizing e

Language: Английский

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Mutual Self-Regulation of d-Electrons of Single Atoms and Adjacent Nanoparticles for Bifunctional Oxygen Electrocatalysis and Rechargeable Zinc-Air Batteries

Nano-Micro Letters, Journal Year: 2023, Volume and Issue: 15(1)

Published: Feb. 11, 2023

Rechargeable zinc-air batteries (ZABs) are a promising energy conversion device, which rely critically on electrocatalysts to accelerate their rate-determining reactions such as oxygen reduction (ORR) and evolution (OER). Herein, we fabricate range of bifunctional M-N-C (metal-nitrogen-carbon) catalysts containing M-Nx coordination sites M/MxC nanoparticles (M = Co, Fe, Cu) using new class γ-cyclodextrin (CD) based metal-organic framework the precursor. With two types active interacting with each other in catalysts, obtained Fe@C-FeNC Co@C-CoNC display superior alkaline ORR activity terms low half-wave (E1/2) potential (~ 0.917 0.906 V, respectively), higher than Cu@C-CuNC 0.829 V) commercial Pt/C 0.861 V). As electrocatalyst, exhibits best performance, showing ORR/OER overpotential (ΔE) ~ 0.732 is much lower that 0.831 1.411 V), well most robust reported date. Synchrotron X-ray absorption spectroscopy density functional theory simulations reveal strong electronic correlation between metallic Co atomic Co-N4 catalyst can increase d-electron near Fermi level thus effectively optimize adsorption/desorption intermediates ORR/OER, resulting an enhanced electrocatalytic performance. The Co@C-CoNC-based rechargeable ZAB exhibited maximum power 162.80 mW cm-2 at 270.30 mA cm-2, combination + RuO2 158.90 265.80 cm-2) catalysts. During galvanostatic discharge 10 delivered almost stable voltage 1.2 V for 140 h, signifying virtue excellent activity.

Language: Английский

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Designing Oxide Catalysts for Oxygen Electrocatalysis: Insights from Mechanism to Application

Nano-Micro Letters, Journal Year: 2023, Volume and Issue: 15(1)

Published: July 29, 2023

Abstract The electrochemical oxygen reduction reaction (ORR) and evolution (OER) are fundamental processes in a range of energy conversion devices such as fuel cells metal–air batteries. ORR OER both have significant activation barriers, which severely limit the overall performance that utilize ORR/OER. Meanwhile, is another very important involving has been widely investigated. occurs aqueous solutions via two pathways: direct 4-electron or 2-electron pathways from O 2 to water (H O) hydrogen peroxide ). Noble metal electrocatalysts often used catalyze ORR, despite fact noble certain intrinsic limitations, low storage. Thus, it urgent develop more active stable low-cost electrocatalysts, especially for severe environments (e.g., acidic media). Theoretically, an ideal electrocatalyst should provide adequate binding species. Transition metals not belonging platinum group metal-based oxides substance could give d orbital species binding. As result, transition regarded substitute typical precious electrocatalysts. However, development oxide catalysts reactions still faces challenges, e.g., catalytic activity, stability, cost, mechanism. We discuss principles underlying design catalysts, including influence crystal structure, electronic structure on their performance. also challenges associated with developing potential strategies overcome these challenges.

Language: Английский

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Operando Scanning Electrochemical Probe Microscopy during Electrocatalysis

Chemical Reviews, Journal Year: 2023, Volume and Issue: 123(8), P. 4972 - 5019

Published: March 27, 2023

Scanning electrochemical probe microscopy (SEPM) techniques can disclose the local reactivity of interfaces in single-entity and sub-entity studies. Operando SEPM measurements consist using a tip to investigate performance electrocatalysts, while interface is simultaneously modulated. This powerful combination correlate activity with changes surface properties, e.g., topography structure, as well provide insight into reaction mechanisms. The focus this review reveal recent progress catalytic toward reduction evolution O2 H2 conversion CO2. capabilities SEPMs are showcased, possibility coupling other presented. Emphasis given scanning (SECM), ion conductance (SICM), tunneling (EC-STM), cell (SECCM).

Language: Английский

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Nitrate induced precise atom substitution and vacancies for overall water splitting

Chemical Engineering Journal, Journal Year: 2023, Volume and Issue: 463, P. 142380 - 142380

Published: March 16, 2023

Language: Английский

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Internal Polarization Field Induced Hydroxyl Spillover Effect for Industrial Water Splitting Electrolyzers

Nano-Micro Letters, Journal Year: 2023, Volume and Issue: 16(1)

Published: Nov. 30, 2023

The formation of multiple oxygen intermediates supporting efficient evolution reaction (OER) are affinitive with hydroxyl adsorption. However, ability the catalyst to capture and maintain continuous supply at active sits remains a tremendous challenge. Herein, an affordable Ni

Language: Английский

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High‐Efficiency Oxygen Evolution Reaction: Controllable Reconstruction of Surface Interface

Small, Journal Year: 2023, Volume and Issue: 19(49)

Published: Aug. 7, 2023

Abstract The precatalyst undergoes surface reconstruction during the oxygen evolution reaction (OER) process, and reconstituted material is one that really plays a catalytic role. However, degree of seriously affects performance. For this reason, it important to establish link between activity based on deep understanding OER mechanism for rational design high‐performance electrocatalysts. Here, briefly introduced, competition adsorbate (AEM) lattice oxygen‐mediated (LOM) discussed, several descriptors are summarized. strategies realize controllable emphatically including ion leaching, element doping, regulating catalyst size, heterogeneous structure engineering, self‐reconstruction. A mechanistic perspective emphasized understand relationship dynamic electronic structure. Controlled reconfiguration can break limitation proportional brought by traditional AEM mechanism, also switching LOM thus realizing ultra‐low overpotential. This review will provide some reference transition metal‐based catalysts reasonable development ideal

Language: Английский

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