A high-entropy atomic environment converts inactive to active sites for electrocatalysis

Energy & Environmental Science, Год журнала: 2023, Номер 16(2), С. 619 - 628

Опубликована: Янв. 1, 2023

An electronegativity-dominant high-entropy atomic environment regulation strategy was developed to manipulate the electrocatalytic properties by tailoring competitive adsorption sites in HEA NPs.

Язык: Английский

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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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High-entropy alloys in electrocatalysis: from fundamentals to applications

Chemical Society Reviews, Год журнала: 2023, Номер 52(23), С. 8319 - 8373

Опубликована: Янв. 1, 2023

In this review, we provide a comprehensive summary of recent advances in the synthesis strategies, design principles, and characterization technologies high entropy alloys, their applications various electrocatalytic conversion reactions.

Язык: Английский

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Mesoporous multimetallic nanospheres with exposed highly entropic alloy sites

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

Опубликована: Июль 13, 2023

Multimetallic alloys (MMAs) with various compositions enrich the materials library increasing diversity and have received much attention in catalysis applications. However, precisely shaping MMAs mesoporous nanostructures mapping distributions of multiple elements remain big challenge due to different reduction kinetics metal precursors complexity crystal growth. Here we design a one-pot wet-chemical approach synthesize core-shell motif PtPdRhRuCu nanospheres (PtPdRhRuCu MMNs) using diblock copolymer as soft template. The MMNs feature adjustable exposed porous structures rich highly entropic alloy sites. formation processes growth are revealed. exhibit robust electrocatalytic hydrogen evolution reaction (HER) activities low overpotentials 10, 13, 28 mV at current density 10 mA cm-2 alkaline (1.0 M KOH), acidic (0.5 H2SO4), neutral phosphate buffer solution (PBS)) electrolytes, respectively. accelerated HER derived from synergistic interactions among sites excellent mass/electron transportation characteristics.

Язык: Английский

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High‐Entropy Alloy Aerogels: A New Platform for Carbon Dioxide Reduction

Advanced Materials, Год журнала: 2022, Номер 35(2)

Опубликована: Ноя. 14, 2022

High-entropy alloy aerogels (HEAAs) combined with the advantages of high-entropy alloys and are prospective new platforms in catalytic reactions. However, due to differences reduction potentials miscibility behavior different metals, realization HEAAs a single phase is still great challenge. Herein, series fabricated via freeze-thaw method as highly active durable electrocatalysts for carbon dioxide reaction (CO2 RR). Especially, PdCuAuAgBiIn can achieve Faradaic efficiency (FE) C1 products almost 100% from -0.7 -1.1 V versus reversible hydrogen electrode (VRHE ), maximum FE formic acid (FEHCOOH ) 98.1% at VRHE , outperforming particles (HEAPs) Pd metallic (MAs). Specifically, current density FEHCOOH 200 mA cm-2 87% flow cell. The impressive CO2 RR performance attributed strong interactions between metals surface unsaturated sites, which regulate electronic structures allow optimal HCOO* intermediate adsorption desorption onto catalysts enhance HCOOH production. work not only provides facile synthetic strategy fabricate HEAAs, but also opens avenue development efficient beyond.

Язык: Английский

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Tuning Mass Transport in Electrocatalysis Down to Sub‐5 nm through Nanoscale Grade Separation

Angewandte Chemie International Edition, Год журнала: 2022, Номер 62(3)

Опубликована: Ноя. 18, 2022

Nano and single-atom catalysis open new possibilities of producing green hydrogen (H2 ) by water electrolysis. However, for the evolution reaction (HER) which occurs at a characteristic rate proportional to potential, fast generation H2 nanobubbles atomic-scale interfaces often leads blockage active sites. Herein, nanoscale grade-separation strategy is proposed tackle mass-transport problem utilizing ordered three-dimensional (3d) interconnected sub-5 nm pores. The results reveal that 3d criss-crossing mesopores with grade separation allow efficient diffusion bubbles along channels. After support ultrafine ruthenium (Ru), are on superior level two-dimensional system maximizing catalyst performance obtained Ru outperforms most other HER catalysts. This work provides potential route fine-tuning few-nanometer mass transport during

Язык: Английский

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

Advanced Functional Materials, Год журнала: 2022, Номер 33(1)

Опубликована: Окт. 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.

Язык: Английский

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Stabilizing Low‐Valence Single Atoms by Constructing Metalloid Tungsten Carbide Supports for Efficient Hydrogen Oxidation and Evolution

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(42)

Опубликована: Сен. 2, 2023

Abstract Designing novel single‐atom catalysts (SACs) supports to modulate the electronic structure is crucial optimize catalytic activity, but rather challenging. Herein, a general strategy proposed utilize metalloid properties of trap and stabilize single‐atoms with low‐valence states. A series supported on surface tungsten carbide (M‐WC x , M=Ru, Ir, Pd) are rationally developed through facile pyrolysis method. Benefiting from WC exhibit weak coordination W C atoms, resulting in formation active centers similar metals. The unique metal‐metal interaction effectively stabilizes single atoms improves orbital energy level distribution sites. As expected, representative Ru‐WC exhibits superior mass activities 7.84 62.52 mg Ru −1 for hydrogen oxidation evolution reactions (HOR/HER), respectively. In‐depth mechanistic analysis demonstrates that an ideal dual‐sites cooperative mechanism achieves suitable adsorption balance H ad OH energetically favorable Volmer step. This work offers new guidance precise construction highly SACs.

Язык: Английский

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High entropy alloy nanoparticles as efficient catalysts for alkaline overall seawater splitting and Zn-air batteries

Journal of Colloid and Interface Science, Год журнала: 2023, Номер 646, С. 844 - 854

Опубликована: Май 17, 2023

Язык: Английский

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High‐Entropy Catalyst—A Novel Platform for Electrochemical Water Splitting

Advanced Functional Materials, Год журнала: 2022, Номер 32(47)

Опубликована: Сен. 16, 2022

Abstract High‐entropy materials (HEMs) have been in the spotlight as emerging catalysts for electrochemical water splitting. In particular, HEM feature multi‐element active sites and unsaturated coordination well entropy stabilization comparison with their single‐element counterparts. Herein, a comprehensive overview of used splitting is provided, covering both hydrogen evolution reaction (HER) oxygen (OER). Particularly, review begins discussions concept structure HEMs. addition, effective strategies rationally designing HEMs on basis computational techniques experimental aspects described. Importantly, importance computationally aided methods, that is, density functional theory calculations, high‐throughput screening, machine learning, to discovery design HEMs, Furthermore, applications field electrolysis are reviewed. Eventually, an outlook regarding prospects future opportunities provided.

Язык: Английский

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