Bifunctional Electrocatalysts for Overall and Hybrid Water Splitting

Chemical Reviews, Год журнала: 2024, Номер 124(7), С. 3694 - 3812

Опубликована: Март 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

Язык: Английский

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Constructing Built‐in Electric Field in Heterogeneous Nanowire Arrays for Efficient Overall Water Electrolysis

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(26)

Опубликована: Апрель 13, 2023

Efficient bifunctional electrocatalysts for hydrogen and oxygen evolution reactions are key to water electrolysis. Herein, we report a built-in electric field (BEF) strategy fabricate heterogeneous nickel phosphide-cobalt nanowire arrays grown on carbon fiber paper (Ni2 P-CoCH/CFP) with large work function difference (ΔΦ) as overall splitting. Impressively, Ni2 P-CoCH/CFP exhibits remarkable catalytic activity obtain 10 mA cm-2 , respectively. Moreover, the assembled lab-scale electrolyzer driven by an AAA battery delivers excellent stability after 50 h electrocatalysis 100 % faradic efficiency. Computational calculations combining experiments reveal interface-induced effect facilitates asymmetrical charge distributions, thereby regulating adsorption/desorption of intermediates during reactions. This offers avenue rationally design high-performance electrocatalysts.

Язык: Английский

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Construction of Zn-doped RuO2 nanowires for efficient and stable water oxidation in acidic media

Nature Communications, Год журнала: 2023, Номер 14(1)

Опубликована: Май 2, 2023

Abstract Oxygen evolution reaction catalysts capable of working efficiently in acidic media are highly demanded for the commercialization proton exchange membrane water electrolysis. Herein, we report a Zn-doped RuO 2 nanowire array electrocatalyst with outstanding catalytic performance oxygen under conditions. Overpotentials as low 173, 304, and 373 mV achieved at 10, 500, 1000 mA cm −2 , respectively, robust stability reaching to h 10 . Experimental theoretical investigations establish clear synergistic effect Zn dopants vacancies on regulating binding configurations oxygenated adsorbates active centers, which then enables an alternative Ru−Zn dual-site oxide path reaction. Due change pathways, energy barrier rate-determining step is reduced, over-oxidation Ru sites alleviated. As result, activity significantly enhanced.

Язык: Английский

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Activating Lattice Oxygen in Layered Lithium Oxides through Cation Vacancies for Enhanced Urea Electrolysis

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(31)

Опубликована: Май 18, 2022

Despite the fact that high-valent nickel-based oxides exhibit promising catalytic activity for urea oxidation reaction (UOR), fundamental questions concerning origin of high performance and structure-activity correlations remain to be elucidated. Here, we unveil underlying enhanced mechanism UOR by employing a series prepared cation-vacancy controllable LiNiO2 (LNO) model catalysts. Impressively, optimized layered LNO-2 exhibits an extremely low overpotential at 10 mA cm-2 along with excellent stability after 160 h test. Operando characterisations combined theoretical analysis reveal activated lattice oxygen in moderate cation vacancies triggers charge disproportion Ni site form Ni4+ species, facilitating deprotonation involved process.

Язык: Английский

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Long‐Term Stability Challenges and Opportunities in Acidic Oxygen Evolution Electrocatalysis

Angewandte Chemie International Edition, Год журнала: 2022, Номер 62(11)

Опубликована: Дек. 22, 2022

Abstract Polymer electrolyte membrane water electrolysis (PEMWE) has been regarded as a promising technology for renewable hydrogen production. However, acidic oxygen evolution reaction (OER) catalysts with long‐term stability impose grand challenge in its large‐scale industrialization. In this review, critical factors that may lead to catalyst's instability couple potential solutions are comprehensively discussed, including mechanical peeling, substrate corrosion, active‐site over‐oxidation/dissolution, reconstruction, oxide crystal structure collapse through the lattice oxygen‐participated pathway, etc. Last but not least, personal prospects provided terms of rigorous evaluation criteria, situ / operando characterizations, economic feasibility and practical electrolyzer consideration, highlighting ternary relationship evolution, industrial‐relevant activity serve roadmap towards ultimate application PEMWE.

Язык: Английский

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Self-Assembly of Ir-Based Nanosheets with Ordered Interlayer Space for Enhanced Electrocatalytic Water Oxidation

Journal of the American Chemical Society, Год журнала: 2022, Номер 144(5), С. 2208 - 2217

Опубликована: Янв. 31, 2022

Iridium (Ir)-based electrocatalysts are widely explored as benchmarks for acidic oxygen evolution reactions (OERs). However, further enhancing their catalytic activity remains challenging due to the difficulty in identifying active species and unfavorable architectures. In this work, we synthesized ultrathin Ir-IrOx/C nanosheets with ordered interlayer space enhanced OER by a nanoconfined self-assembly strategy, employing block copolymer formed stable end-merged lamellar micelles. The distance of prepared was well controlled at ∼20 nm Ir-IrOx nanoparticles (∼2 nm) were uniformly distributed within nanosheets. Importantly, fabricated display one lowest overpotential (η) 198 mV 10 mA cm-2geo during an acid medium, benefiting from features mixed-valence states, rich electrophilic (O(II-δ)-), favorable mesostructured Both experimental computational results reveal that mixed valence O(II-δ)- moieties 2D mesoporous catalysts shortened Ir-O(II-δ)- bond (1.91 Å) is key enhancement balancing adsorption free energy oxygen-containing intermediates. This strategy thus opens avenue designing high performance through water oxidation beyond.

Язык: Английский

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Atomically precise electrocatalysts for oxygen reduction reaction

Chem, Год журнала: 2023, Номер 9(2), С. 280 - 342

Опубликована: Фев. 1, 2023

Язык: Английский

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

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(43)

Опубликована: Сен. 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

Язык: Английский

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Recent progress and perspective of cobalt-based catalysts for water splitting: design and nanoarchitectonics

Materials Today Energy, Год журнала: 2021, Номер 23, С. 100911 - 100911

Опубликована: Ноя. 26, 2021

Язык: Английский

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Hierarchically Ordered Macro–Mesoporous Electrocatalyst with Hydrophilic Surface for Efficient Oxygen Reduction Reaction

Advanced Materials, Год журнала: 2023, Номер 35(30)

Опубликована: Апрель 18, 2023

Metal-organic frameworks (MOFs) offer versatile templates/precursors to prepare supported metal catalysts. However, the afforded catalysts usually exhibit microporous structures and unsuitable wettability, which will restrict accessibility of active sites in liquid-phase reactions. Herein, an etching-functionalization strategy is developed for construction a tannic-acid-functionalized MOF with unique hollow-wall 3D-ordered macroporous (H-3DOM) structure. The functional can be further employed as ideal precursor synthesis cobalt on oxygen/nitrogen-co-doped carbon composites H-3DOM structures, hydrophilic surface. structure improve external surface area maximize exposure sites. Moreover, oxygen-containing groups enhance wettability guarantee more electrochemically accessible aqueous electrolyte. Benefitting from these outstanding characteristics, H-3DOM-Co/ONC exhibits high electrocatalytic activity oxygen reduction reaction, superior its counterparts without hierarchically ordered functionalization.

Язык: Английский

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