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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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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Unraveling the electronegativity-dominated intermediate adsorption on high-entropy alloy electrocatalysts

Nature Communications, Journal Year: 2022, Volume and Issue: 13(1)

Published: May 13, 2022

Abstract High-entropy alloys have received considerable attention in the field of catalysis due to their exceptional properties. However, few studies hitherto focus on origin outstanding performance and accurate identification active centers. Herein, we report a conceptual experimental approach overcome limitations single-element catalysts by designing FeCoNiXRu (X: Cu, Cr, Mn) system with various sites that different adsorption capacities for multiple intermediates. The electronegativity differences between mixed elements HEA induce significant charge redistribution create highly Co Ru optimized energy barriers simultaneously stabilizing OH * H intermediates, which greatly enhances efficiency water dissociation alkaline conditions. This work provides an in-depth understanding interactions specific opens up fascinating direction breaking scaling relation issues multistep reactions.

Language: Английский

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High Entropy Alloy Electrocatalytic Electrode toward Alkaline Glycerol Valorization Coupling with Acidic Hydrogen Production

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 144(16), P. 7224 - 7235

Published: April 11, 2022

Electrochemical glycerol oxidation reaction (GOR) is an attractive alternative anodic to oxygen evolution for a variety of electrolytic synthesis, thanks the possibility mass production from biomass and relative low thermodynamic potential GOR. The development high-activity cheap electrocatalysts toward GOR yet faces daunting challenge. Herein, we experimentally prepare new range high entropy alloy (HEA) self-supported electrodes with uniform HEA nanoparticles grown on carbon cloth. systematic electrochemical studies verify that HEA-CoNiCuMnMo electrode exhibits performance electrocatalysis overpotential selectivity formate products. surface atomic configurations are studied by self-developed machine learning-based Monte Carlo simulation, which points out catalytic active center be Mo sites coordinated Mn, Mo, Ni. We further develop hybrid alkali/acid flow cell pairing alkaline acidic hydrogen using commercial RhIr/Ti as anode cathode, respectively, only requires applied voltage 0.55 V reach current density 10 mA cm-2 maintains long-term electrolysis stability over 12 days continuous running at 50 Faraday efficiencies 99% H2 in cathode 92% anode.

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 comprehensive review on the electrochemical parameters and recent material development of electrochemical water splitting electrocatalysts

RSC Advances, Journal Year: 2023, Volume and Issue: 13(6), P. 3843 - 3876

Published: Jan. 1, 2023

Electrochemical splitting of water is an appealing solution for energy storage and conversion to overcome the reliance on depleting fossil fuel reserves prevent severe deterioration global climate. Though there are several cells, hydrogen (H

Language: Английский

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Self‐Reconstruction of Sulfate‐Containing High Entropy Sulfide for Exceptionally High‐Performance Oxygen Evolution Reaction Electrocatalyst

Advanced Functional Materials, Journal Year: 2021, Volume and Issue: 31(48)

Published: Aug. 31, 2021

Abstract Novel earth‐abundant metal sulfate‐containing high entropy sulfides, FeNiCoCrXS 2 (where X = Mn, Cu, Zn, or Al), are synthesized via a two‐step solvothermal method. It is shown that FeNiCoCrMnS exhibits superior oxygen evolution reaction (OER) activity with an exceptionally low overpotential of 199, 246, 285, and 308 mV at current densities 10, 100, 500, 1000 mA cm –2 , respectively, surpassing its unary‐, binary‐, ternary‐, quaternary‐metal counterparts. The electrocatalyst yields exceptional stability after 12 000 cycles 55 h durability even density 500 . Various in situ ex analyses used to investigate the self‐reconstruction sulfides during OER for first time. resulting (oxy)hydroxide believed be true active center OER. remaining sulfate also contributes catalytic activity. Density function theory calculation good agreement experimental result. extraordinary performance sulfide brings great opportunity desirable catalyst design practical applications.

Language: Английский

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High-entropy single-atom activated carbon catalysts for sustainable oxygen electrocatalysis

Nature Sustainability, Journal Year: 2023, Volume and Issue: 6(7), P. 816 - 826

Published: March 30, 2023

Language: Английский

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High‐Entropy Atomic Layers of Transition‐Metal Carbides (MXenes)

Advanced Materials, Journal Year: 2021, Volume and Issue: 33(39)

Published: Aug. 8, 2021

Abstract High‐entropy materials (HEMs) have great potential for energy storage and conversion due to their diverse compositions, unexpected physical chemical features. However, high‐entropy atomic layers with fully exposed active sites are difficult synthesize since phases easily segregated. Here, it is demonstrated that of transition‐metal carbide (HE‐MXene) can be produced via the selective etching novel MAX (also termed M n +1 AX ( = 1, 2, 3), where represents an early element, A element mainly from groups 13–16, X stands C and/or N) phase (HE‐MAX) (Ti 1/5 V Zr Nb Ta ) 2 AlC, in which five species homogeneously dispersed into one MX slab solid‐solution feature, giving rise a stable owing high molar configurational entropy correspondingly low Gibbs free energy. Additionally, resultant MXene distinct lattice distortions leads mechanical strain layers. Moreover, efficiently guide nucleation uniform growth dendrite‐free lithium on HE‐MXene, achieving long cycling stability up 1200 h good deep stripping–plating levels 20 mAh cm −2 .

Language: Английский

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High Configuration Entropy Activated Lattice Oxygen for O₂ Formation on Perovskite Electrocatalyst

Advanced Functional Materials, Journal Year: 2022, Volume and Issue: 32(28)

Published: April 13, 2022

Abstract The single‐phase oxides with elemental complexity and compositional diversity, usually named high entropy oxides, feature homogeneously dispersed multi‐metallic elements in equiatomic concentration. unusual properties of endow their potential application clean‐energy‐related electrocatalysis. However, the possible fundamental relationship between configuration underlying catalytic mechanism is still not well understood established. Herein, a perovskite cobaltate consisting five equimolar metals B‐site (Mg, Mn, Fe, Co, Ni) employed as an electrocatalyst for oxygen evolution reaction (OER). serves effective tool to promote intrinsic activity Co reactive site manipulate OER mechanism. demonstrates lower overpotential 320 mV at current density 10 mA cm −2 , outperforming other counterparts. X‐ray spectroscopies disclose synergistic charge‐exchange effect among different cations formation new hole state. Combinatorially computational experimental results unveil enigma that leads random occupation cations, facilitates surface reconstruction, benefits stable vacancies. Owing these merits, O 2 found be kinetically favorable via lattice

Language: Английский

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