Bifunctional Electrocatalysts for Overall and Hybrid Water Splitting

Chemical Reviews, Journal Year: 2024, Volume and Issue: 124(7), P. 3694 - 3812

Published: March 22, 2024

Electrocatalytic water splitting driven by renewable electricity has been recognized as a promising approach for green hydrogen production. Different from conventional strategies in developing electrocatalysts the two half-reactions of (e.g., and oxygen evolution reactions, HER OER) separately, there growing interest designing bifunctional electrocatalysts, which are able to catalyze both OER. In addition, considering high overpotentials required OER while limited value produced oxygen, is another rapidly exploring alternative oxidation reactions replace hybrid toward energy-efficient generation. This Review begins with an introduction on fundamental aspects splitting, followed thorough discussion various physicochemical characterization techniques that frequently employed probing active sites, emphasis reconstruction during redox electrolysis. The design, synthesis, performance diverse based noble metals, nonprecious metal-free nanocarbons, overall acidic alkaline electrolytes, thoroughly summarized compared. Next, their application also presented, wherein anodic include sacrificing agents oxidation, pollutants oxidative degradation, organics upgrading. Finally, concise statement current challenges future opportunities presented hope guiding endeavors quest sustainable

Language: Английский

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Enlarging the Ni–O Bond Polarizability in a Phosphorene-Hosted Metal–Organic Framework for Boosted Water Oxidation Electrocatalysis

ACS Nano, Journal Year: 2023, Volume and Issue: 17(17), P. 17254 - 17264

Published: Aug. 31, 2023

The emerging lattice-oxygen oxidation mechanism (LOM) presents attractive opportunities for breaking the scaling relationship to boost oxygen evolution reaction (OER) with direct OLattice-*O interaction. However, currently LOM-triggering rationales are still debated, and a streamlined physicochemical paradigm is extremely desirable design of LOM-defined OER catalysts. Herein, Ni metal-organic framework/black phosphorene (NiMOF/BP) heterostructure theoretically profiled constructed as catalytic platform LOM-derived studies. It found that p-type BP host can enlarge Ni-O bond polarizability NiMOF through stretching valence declining synergically. Such an enlarged will in principle alleviate lattice confinement benefit LOM pathway performance. As result, optimized NiMOF/BP catalyst exhibits promising performance low overpotential 260 mV at 10 mA cm-2 long-term stability 1 M KOH electrolyte. Both experiment calculation results suggest activated more balanced step barrier catalyst. This research puts forward criterion LOM-scaled electrocatalysts water oxidation.

Language: Английский

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Asymmetric Bond Delta‐Polarization at the Interfacial Se─Ru─O Bridge for Efficient pH‐Robust Water Electrolysis

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: June 10, 2024

Abstract The rationalization of pH‐robust catalysis is highly desired but challengeable for overall water electrolysis (WE). It requests a metal active site that can make an efficient adaption with both cathodic hydrogen and anodic oxygen evolution reactions (HER/OER). Herein, RuO 2‐x /RuSe 2 heterostructure electrocatalyst profiled interfacial Se─Ru─O bridge the splitting studies. An asymmetric bond delta‐polarization (Δp) found at bridge, including Δp > 0 Ru─O part < Ru─Se side by experiment calculation results. enlarged polarizability (Δp 0) in principle trigger lattice mediated (LOM) pathway OER; meanwhile, reduced benefit HER due to strengthened d‐p band hybridization. Resultantly, deliver ultralow overpotentials 25/10 mV Pt‐beyond 210/255 OER 10 mA cm −2 acidic/alkaline media, respectively. In especial, acidic WE be stably operated 200 h low cell voltage 1.478 V . This research clarifies polarization as criterion rational design catalysts.

Language: Английский

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Stability challenges and opportunities of NiFe‐based electrocatalysts for oxygen evolution reaction in alkaline media

Carbon Neutralization, Journal Year: 2024, Volume and Issue: 3(2), P. 172 - 198

Published: Feb. 26, 2024

Abstract Water splitting is a critical process for the production of green hydrogen, contributing to advancement circular economy. However, application water devices on large scale primarily impeded by sluggish oxygen evolution reaction (OER) at anode. Thus, developing and designing efficient OER catalysts significant target. NiFe‐based are extensively researched as excellent electrocatalysts due their affordability, abundant reserves, intrinsic activities. they still suffer from long‐term stability challenges. To date, few systematic strategies improving durability have been reported. In this review, various advanced introduced. Moreover, challenges in alkaline media, including iron segregation, structural degradation, peeling substrate summarized. More importantly, enhance highlighted opportunities discussed facilitate future studies electrolysis. This review presents design strategy anion exchange membrane (AEM) electrolyzers overcome OER, which also emphasizes importance media its significance achieving large‐scale commercialization.

Language: Английский

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NiFe-Based Semi-MOF Embedded by Sulfide Particles Reconstructed a Three-Layer Sandwich Structure for Alkaline Overall Water Splitting

ACS Sustainable Chemistry & Engineering, Journal Year: 2024, Volume and Issue: 12(11), P. 4551 - 4564

Published: March 1, 2024

A metal–organic framework (MOF) embedded by transition metal sulfide (TMS) particles is one of the promising electrocatalyst candidates for overall water splitting (OWS) due to large surface area and abundant active sites from MOF precursor, as well tunable electronic structure higher intrinsic conductivity TMS. More importantly, its self-restructuring under alkaline conditions will lead chemical composition phase evolution catalyst surface, which source further enhanced catalytic activity. semi-MOF (labeled Co@Ni/Fe-MS/MOF) with semisacrificial template a TMS particle guest was designed exercisable universal heteroatomic Co doping partial vulcanization. The TMS/MOF heterostructure establishes an ideal bridge electron transfer. Simultaneously, dopant synergistic effect multiple also effectively regulate charge environment around sites, jointly improve adsorption/desorption kinetics reaction intermediates. As result, Co@Ni/Fe-MS/MOF exhibits distinguished overpotential (η10 = 229 mV OER, η10 174 HER) Tafel slope (52.37/114.35 dec–1 OER/HER), unrivaled long-term durability (80 h OWS). Moreover, two-electrode ∥ cell illustrates small voltage 1.54 V achieve power 10 mA cm–2. Impressively, this superior OER property comes three-layer sandwich restructured hybrid semi-MOFs in true sites. This work aspired catalyst, induce effects, shed light on preparation materials heterogeneous interface engineering, evolution.

Language: Английский

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Engineering metal-organic frameworks-based nanozymes for enhanced biomimetic catalytic sensing

TrAC Trends in Analytical Chemistry, Journal Year: 2024, Volume and Issue: 178, P. 117862 - 117862

Published: July 10, 2024

Language: Английский

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Thiosalicylic‐Acid‐Mediated Coordination Structure of Nickel Center via Thermodynamic Modulation for Aqueous Ni–Zn Batteries

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(32)

Published: May 30, 2024

Uniquely functional nanocomplexes with rich coordination environments are critical in energy storage. However, the construction of structurally versatile remains challenging. In this study, a nickel-based complex structural variations is designed via thermodynamic modulation using dual-ligand synthesis strategy. A nanomaterial (NiSA-SSA-160) large specific surface area synthesized around competing host and guest molecules that differ terms chemical properties O S elements. Concurrently, environment NiSA-SSA-160 investigated X-ray absorption fine structure spectroscopy. The thiol groups synergistically induced an electron-rich Ni structure, thus increasing electron density central atom. electrochemical performance assembled NiSA-SSA-160//Zn@CC battery shown to improve significantly, maximum 0.54 mWh cm

Language: Английский

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Construction of 2D CoFe-MOF derived from LDH electrocatalyst for efficient oxygen and urea evolution

Journal of Colloid and Interface Science, Journal Year: 2025, Volume and Issue: 684, P. 243 - 250

Published: Jan. 15, 2025

Language: Английский

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MOF-Based Electrocatalysts: An Overview from the Perspective of Structural Design

Chemical Reviews, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 18, 2025

The electrocatalytic technique, as an efficient energy storage and conversion technology, has attracted significant attention to address exhaustion environmental pollution. Usually, the activity selectivity of reactions are largely dominated by dynamic process occurring on electrocatalysts. Therefore, high-performance electrocatalysts, which can dominate pathway barrier reactions, great significance for advancement technique. Metal-organic frameworks (MOFs), emerging crystalline porous materials, present structural component advantages including well-defined structure, high surface area, large porosity, diverse components, easy tailorability, demonstrating fantastic potential precise fabrication In this Review, strategies in electrocatalysts based MOF-related materials specifically introduced from aspects catalytic site design microenvironment modulation around sites. Furthermore, representative progress achieved various applications employing MOF-based is systematically summarized, with special emphasis MOFs performance optimization. Finally, remaining challenges future perspectives further highlighted.

Language: Английский

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Molecular Engineering of a Metal‐Organic Polymer for Enhanced Electrochemical Nitrate‐to‐Ammonia Conversion and Zinc Nitrate Batteries

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(48)

Published: Oct. 13, 2023

Metal-organic framework-based materials are promising single-site catalysts for electrocatalytic nitrate (NO3- ) reduction to value-added ammonia (NH3 on account of well-defined structures and functional tunability but still lack a molecular-level understanding designing the high-efficient catalysts. Here, we proposed molecular engineering strategy enhance electrochemical NO3- -to-NH3 conversion by introducing carbonyl groups into 1,2,4,5-tetraaminobenzene (BTA) based metal-organic polymer precisely modulate electronic state metal centers. Due electron-withdrawing properties group, centers can be converted an electron-deficient state, fascinating adsorption promoting continuous hydrogenation reactions produce NH3 . Compared CuBTA with low efficiency 85.1 %, quinone group functionalization endows resulting copper tetraminobenzoquinone (CuTABQ) distinguished performance much higher FE 97.7 %. This is also universal, as verified improved different centers, including Co Ni. Furthermore, assembled rechargeable Zn-NO3- battery CuTABQ cathode deliver high power density 12.3 mW cm-2 work provides advanced insights rational design complex through regulation electroreduction

Language: Английский

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