High-entropy nanoparticles: Synthesis-structure-property relationships and data-driven discovery

Science, Journal Year: 2022, Volume and Issue: 376(6589)

Published: April 7, 2022

High-entropy nanoparticles have become a rapidly growing area of research in recent years. Because their multielemental compositions and unique high-entropy mixing states (i.e., solid-solution) that can lead to tunable activity enhanced stability, these received notable attention for catalyst design exploration. However, this strong potential is also accompanied by grand challenges originating from vast compositional space complex atomic structure, which hinder comprehensive exploration fundamental understanding. Through multidisciplinary view synthesis, characterization, catalytic applications, high-throughput screening, data-driven materials discovery, review dedicated discussing the important progress unveiling critical needs future development catalysis, energy, sustainability applications.

Language: Английский

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High-entropy materials for catalysis: A new frontier

Science Advances, Journal Year: 2021, Volume and Issue: 7(20)

Published: May 12, 2021

Entropy plays a pivotal role in catalysis, and extensive research efforts have been directed to understanding the enthalpy-entropy relationship that defines reaction pathways of molecular species. On other side, surface catalysts, entropic effects rarely investigated because difficulty deciphering increased complexities multicomponent systems. Recent advances high-entropy materials (HEMs) triggered broad interests exploring entropy-stabilized systems for where enhanced configurational entropy affords virtually unlimited scope tailoring structures properties HEMs. In this review, we summarize recent progress discovery design HEMs catalysis. The correlation between compositional structural engineering optimization catalytic behaviors is highlighted alloys, oxides, beyond. Tuning composition configuration introduces untapped opportunities accessing better catalysts resolving issues are considered challenging conventional, simple

Language: Английский

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Subnanometer high-entropy alloy nanowires enable remarkable hydrogen oxidation catalysis

Nature Communications, Journal Year: 2021, Volume and Issue: 12(1)

Published: Oct. 29, 2021

High-entropy alloys (HEAs) with unique physicochemical properties have attracted tremendous attention in many fields, yet the precise control on dimension and morphology at atomic level remains formidable challenges. Herein, we synthesize PtRuNiCoFeMo HEA subnanometer nanowires (SNWs) for alkaline hydrogen oxidation reaction (HOR). The mass specific activities of SNWs/C reach 6.75 A mgPt+Ru-1 8.96 mA cm-2, respectively, which are 2.8/2.6, 4.1/2.4, 19.8/18.7 times higher than those NPs/C, commercial PtRu/C Pt/C, respectively. It can even display enhanced resistance to CO poisoning during HOR presence 1000 ppm CO. Density functional theory calculations reveal that strong interactions between different metal sites SNWs greatly regulate binding strength proton hydroxyl, therefore enhances activity. This work not only provides a viable synthetic route fabrication Pt-based subnano/nano materials, but also promotes fundamental researches catalysis beyond.

Language: Английский

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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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Multi‐Sites Electrocatalysis in High‐Entropy Alloys

Advanced Functional Materials, Journal Year: 2021, Volume and Issue: 31(47)

Published: Aug. 26, 2021

Abstract High‐entropy alloys (HEAs) have attracted widespread attention in electrocatalysis due to their unique advantages (adjustable composition, complex surface, high tolerance, etc.). They allow for the formation of new and tailorable active sites multiple elements adjacent each other, interaction can be tailored by rational selection element configuration composition. However, it needs further explored catalyst design, elements, determination sites. This review article focuses on important progress multi‐sites HEAs. The classification is done basis catalytic reaction, including hydrogen evolution oxygen reduction alcohol oxidation carbon dioxide nitrogen reaction. Based experiments theories, a more in‐depth exploration activity HEAs will conducted, (the special role catalysis) effect. provide design some reactions, adjust compositions improve intrinsic activity. Furthermore, remaining challenges future directions promising research fields are also provided.

Language: Английский

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High‐Entropy Prussian Blue Analogues and Their Oxide Family as Sulfur Hosts for Lithium‐Sulfur Batteries

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(41)

Published: Aug. 25, 2022

The introduction of high-entropy into Prussian blue analogues (PBAs) has yet to attract attention in the field lithium-sulfur battery materials. Herein, we systematically synthesize a library PBAs from binary by facile coprecipitation method. coordination environment is explored X-ray absorption fine structure spectroscopy, which together with elemental mapping confirm successful all metals. Importantly, electrochemical tests demonstrate that PBA can serve as polysulfide immobilizer inhibit shuttle effect and catalyst promote polysulfides conversion, thereby boosting its outstanding performance. Additionally, variety nanocubic metal oxides senary are fabricated using sacrificial precursors. We believe wide range new materials obtained our pyrolysis methodology further developments research on systems sulfur hosts.

Language: Английский

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Ultrahigh Stable Methanol Oxidation Enabled by a High Hydroxyl Concentration on Pt Clusters/MXene Interfaces

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 144(34), P. 15529 - 15538

Published: Aug. 9, 2022

Anchoring platinum catalysts on appropriate supports, e.g., MXenes, is a feasible pathway to achieve desirable anode for direct methanol fuel cells. The authentic performance of Pt often hindered by the occupancy and poisoning active sites, weak interaction between dissolution Pt. Herein, we construct three-dimensional (3D) crumpled Ti3C2Tx MXene balls with abundant Ti vacancies confinement via spray-drying process. as-prepared clusters/Ti3C2Tx (Ptc/Ti3C2Tx) show enhanced electrocatalytic oxidation reaction (MOR) activity, including relatively low overpotential, high tolerance CO poisoning, ultrahigh stability. Specifically, it achieves mass activity up 7.32 A mgPt-1, which highest value reported date in Pt-based electrocatalysts, 42% current density retained Ptc/Ti3C2Tx even after 3000 min operative time. In situ spectroscopy theoretical calculations reveal that an electric field-induced repulsion interface accelerates combination OH- adsorption intermediates (COads) kinetics thermodynamics. Besides, this also efficiently electrocatalyze ethanol, ethylene glycol, glycerol reactions comparable stability commercial Pt/C.

Language: Английский

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Solvent-free microwave synthesis of ultra-small Ru-Mo2C@CNT with strong metal-support interaction for industrial hydrogen evolution

Nature Communications, Journal Year: 2021, Volume and Issue: 12(1)

Published: June 29, 2021

Abstract Exploring a simple, fast, solvent-free synthetic method for large-scale preparation of cheap, highly active electrocatalysts industrial hydrogen evolution reaction is one the most promising work today. In this work, fast and microwave pyrolysis used to synthesize ultra-small (3.5 nm) Ru-Mo 2 C@CNT catalyst with heterogeneous structure strong metal-support interaction in step. The only exhibits an overpotential 15 mV at current density 10 mA cm −2 , large turnover frequency value up 21.9 s −1 under 100 1.0 M KOH. addition, can reach high densities 500 1000 low overpotentials 56 78 respectively, it displays stability h. This provides feasible way reasonable design other production catalysts.

Language: Английский

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Electrochemical Nitrate Reduction: Ammonia Synthesis and the Beyond

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(17)

Published: June 9, 2023

Natural nitrogen cycle has been severely disrupted by anthropogenic activities. The overuse of N-containing fertilizers induces the increase nitrate level in surface and ground waters, substantial emission oxides causes heavy air pollution. Nitrogen gas, as main component air, used for mass ammonia production over a century, providing enough nutrition agriculture to support world population increase. In last decade, researchers have made great efforts develop processes under ambient conditions combat intensive energy consumption high carbon associated with Haber-Bosch process. Among different techniques, electrochemical reduction reaction (NO

Language: Английский

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High-entropy alloy stabilized active Ir for highly efficient acidic oxygen evolution

Chemical Engineering Journal, Journal Year: 2021, Volume and Issue: 431, P. 133251 - 133251

Published: Oct. 31, 2021

Language: Английский

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