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

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(2), P. 619 - 628

Published: Jan. 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.

Language: Английский

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The reformation of catalyst: From a trial-and-error synthesis to rational design

Nano Research, Journal Year: 2023, Volume and Issue: 17(4), P. 3261 - 3301

Published: Sept. 27, 2023

Language: Английский

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High‐Entropy Intermetallic PtRhBiSnSb Nanoplates for Highly Efficient Alcohol Oxidation Electrocatalysis

Advanced Materials, Journal Year: 2022, Volume and Issue: 34(43)

Published: Sept. 5, 2022

The control of multimetallic ensembles at the atomic-level is challenging, especially for high-entropy alloys (HEAs) possessing five or more elements. Herein, one-pot synthesis hexagonal-close-packed (hcp) PtRhBiSnSb intermetallic (HEI) nanoplates with intrinsically isolated Pt, Rh, Bi, Sn, and Sb atoms reported, to boost electrochemical oxidation liquid fuels. Taking advantage these combined metals, well-defined HEI exhibit a remarkable mass activity 19.529, 15.558, 7.535 A mg-1Pt+Rh toward electrooxidation methanol, ethanol, glycerol in alkaline electrolytes, respectively, representing state-of-the-art multifunctional electrocatalyst alcohol reactions. In particular, achieves record-high methanol reaction (MOR) an environment. Theoretical calculations demonstrate that introduction fifth metal Rh enhances electron-transfer efficiency nanoplates, which contributes improved capability. Meanwhile, robust electronic structures active sites are achieved due synergistic protections from sites. This work offers significant research advances developing HEA delicate over compositions properties.

Language: Английский

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Toward Electrocatalytic Methanol Oxidation Reaction: Longstanding Debates and Emerging Catalysts

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(26)

Published: Jan. 27, 2023

The study of direct methanol fuel cells (DMFCs) has lasted around 70 years, since the first investigation in early 1950s. Though enormous effort been devoted this field, it is still far from commercialization. oxidation reaction (MOR), as a semi-reaction DMFCs, bottleneck that restricts overall performance DMFCs. To date, there intense debate on complex six-electron reaction, but barely any reviews have systematically discussed topic. end, controversies and progress regarding electrocatalytic mechanisms, evaluations well design science toward MOR electrocatalysts are summarized. This review also provides comprehensive introduction recent development emerging with focus innovation alloy, core-shell structure, heterostructure, single-atom catalysts. Finally, perspectives future outlook mechanisms provided.

Language: Английский

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Clarifying the four core effects of high-entropy materials

Nature Reviews Chemistry, Journal Year: 2024, Volume and Issue: 8(6), P. 471 - 485

Published: May 2, 2024

Language: Английский

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High-entropy alloys in electrocatalysis: from fundamentals to applications

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(23), P. 8319 - 8373

Published: Jan. 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.

Language: Английский

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Mesoporous multimetallic nanospheres with exposed highly entropic alloy sites

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: July 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.

Language: Английский

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

Advanced Materials, Journal Year: 2022, Volume and Issue: 35(2)

Published: Nov. 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.

Language: Английский

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Short‐Range Diffusion Enables General Synthesis of Medium‐Entropy Alloy Aerogels

Advanced Materials, Journal Year: 2022, Volume and Issue: 34(30)

Published: May 25, 2022

Medium-entropy alloy aerogels (MEAAs) with the advantages of both multimetallic alloys and are promising new materials in catalytic applications. However, limited by immiscible behavior different metals, achieving single-phase MEAAs is still a grand challenge. Herein, general strategy for preparing ultralight 3D porous lowest density 39.3 mg cm-3 among metal reported, through combining auto-combustion subsequent low-temperature reduction procedures. The homogenous mixing precursors at ionic level makes short-range diffusion atoms possible to drive formation MEAAs. As proof concept catalysis, as-synthesized Ni50 Co15 Fe30 Cu5 exhibit high mass activity 1.62 A mg-1 specific 132.24 mA cm-2 toward methanol oxidation reactions, much higher than those low-entropy counterparts. In situ Fourier transform infrared NMR spectroscopies reveal that can enable highly selective conversion formate. Most importantly, methanol-oxidation-assisted MEAAs-based water electrolyzer achieve low cell voltage 1.476 V 10 making value-added formate anode H2 cathode, 173 mV lower traditional alkaline electrolyzers.

Language: Английский

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High-entropy oxides for catalysis: A diamond in the rough

Chemical Engineering Journal, Journal Year: 2022, Volume and Issue: 451, P. 138659 - 138659

Published: Aug. 17, 2022

Language: Английский

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