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 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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High‐Entropy Enhanced Microwave Attenuation in Titanate Perovskites

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(11)

Published: Jan. 6, 2023

High-entropy oxides (HEOs), which incorporate multiple-principal cations into single-phase crystals and interact with diverse metal ions, extend the border for available compositions unprecedented properties. Herein, a high-entropy-stabilized (Ca0.2 Sr0.2 Ba0.2 La0.2 Pb0.2 )TiO3 perovskite is reported, effective absorption bandwidth (90% absorption) improves almost two times than that of BaTiO3 . The results demonstrate regulation entropy configuration can yield significant grain boundaries, oxygen defects, an ultradense distorted lattice. These characteristics give rise to strong interfacial defect-induced polarizations, thus synergistically contributing dielectric attenuation performance. Moreover, large strains derived from lattice distortions in high-entropy offer varied transport electron carriers. high-entropy-enhanced positive/negative charges accumulation around boundaries strain-concentrated location, quantitatively validated by holography, unusual polarization loss. This study opens up avenue designing microwave materials satisfy increasingly demanding requirements advanced integrated electronics. work also offers paradigm improving other interesting properties HEOs through engineering.

Language: Английский

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CHGNet as a pretrained universal neural network potential for charge-informed atomistic modelling

Nature Machine Intelligence, Journal Year: 2023, Volume and Issue: 5(9), P. 1031 - 1041

Published: Sept. 14, 2023

Abstract Large-scale simulations with complex electron interactions remain one of the greatest challenges for atomistic modelling. Although classical force fields often fail to describe coupling between electronic states and ionic rearrangements, more accurate ab initio molecular dynamics suffers from computational complexity that prevents long-time large-scale simulations, which are essential study technologically relevant phenomena. Here we present Crystal Hamiltonian Graph Neural Network (CHGNet), a graph neural network-based machine-learning interatomic potential (MLIP) models universal energy surface. CHGNet is pretrained on energies, forces, stresses magnetic moments Materials Project Trajectory Dataset, consists over 10 years density functional theory calculations than 1.5 million inorganic structures. The explicit inclusion enables learn accurately represent orbital occupancy electrons, enhancing its capability both atomic degrees freedom. We demonstrate several applications in solid-state materials, including charge-informed Li x MnO 2 , finite temperature phase diagram FePO 4 diffusion garnet conductors. highlight significance charge information capturing appropriate chemistry provide insights into systems additional freedom cannot be observed by previous MLIPs.

Language: Английский

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High‐Entropy Alloys for Electrocatalysis: Design, Characterization, and Applications

Small, Journal Year: 2021, Volume and Issue: 18(7)

Published: Nov. 5, 2021

Abstract High‐entropy alloys (HEAs) are expected to function well as electrocatalytic materials, owing their widely adjustable composition and unique physical chemical properties. Recently, HEA catalysts extensively studied in the field of electrocatalysis; this motivated authors investigate relationship between structure HEAs performance. In review, latest advances electrocatalysts systematically summarized, with special focus on nitrogen fixation, carbon cycle, water splitting, fuel cells; addition, by combining characterization analysis microstructures, rational design strategies for optimizing electrocatalysts, including controllable preparation, component regulation, strain engineering, defect theoretical prediction proposed. Moreover, existing issues future trends predicted, which will help further develop these high‐entropy materials.

Language: Английский

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A perspective on the catalysis using the high entropy alloys

Nano Energy, Journal Year: 2021, Volume and Issue: 88, P. 106261 - 106261

Published: June 18, 2021

Language: Английский

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Liquid metal for high-entropy alloy nanoparticles synthesis

Nature, Journal Year: 2023, Volume and Issue: 619(7968), P. 73 - 77

Published: June 14, 2023

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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High-entropy materials for energy and electronic applications

Nature Reviews Materials, Journal Year: 2024, Volume and Issue: 9(4), P. 266 - 281

Published: March 6, 2024

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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