Classics of the Masters

Multiscale Synthesis and Performance Regulation Mechanisms of High-Entropy Materials

  • HAN Jiecai ,
  • SONG Bo ,
  • XU Ping ,
  • XU Yifei ,
  • WANG Kaixi
Expand
  • 1.Center for Composite Materials and Structure, School of Astronautics, Harbin Institute of Technology, Harbin 150001, China
    2.Zhengzhou Advanced Research Institute, Harbin Institute of Technology, Zhengzhou 450000, China
    3.School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150001, China

Received date: 2025-12-09

  Revised date: 2026-01-07

  Online published: 2026-01-09

Supported by

National Science Fund for Distinguished Young Scholars(52225201)

Abstract

Metals and their compounds are core materials in energy catalysis; however, their performance is often constrained by conventional few-component systems, which typically feature single active sites and limited electronic-structure tunability. These limitations hinder precise regulation of complex reaction pathways and product selectivity. High-entropy strategies offer a promising route to overcome these challenges by enabling multi-element synergistic effects. Nevertheless, introducing multiple elements increases the tendency toward phase separation, making the controllable synthesis of single-phase, compositionally uniform high-entropy materials a key bottleneck for practical applications. To address this issue, this study develops a series of controllable synthesis strategies for high-entropy alloys, high-entropy ceramics, and two-dimensional (2D) high-entropy phosphorus trichalcogenides. Specifically, melt extraction is employed to fabricate high-entropy alloy fibers; pressureless sintering is used to synthesize dense high-entropy metal carbides; solid-state synthesis combined with ultrasonic exfoliation enables the production of 2D high-entropy phosphorus trichalcogenides; and a metal-organic framework-derived strategy is adopted to construct high-entropy metal oxides. These methods enable key advances in high-entropy material synthesis, particularly in compositional homogenization, structural densification, dimensional control, and precursor design. Moreover, the role of high-entropy engineering in regulating catalytic performance is systematically elucidated, highlighting the critical contributions of multicomponent synergy to basal-plane activation, optimization of metal—oxygen covalency, and enhancement of structural stability. Overall, this study aims to provide practical technical pathways and a theoretical framework for developing high-performance high-entropy materials through innovative synthesis strategies and in-depth mechanistic insights.

Cite this article

HAN Jiecai , SONG Bo , XU Ping , XU Yifei , WANG Kaixi . Multiscale Synthesis and Performance Regulation Mechanisms of High-Entropy Materials[J]. Acta Metall Sin, 2026 , 62(3) : 397 -405 . DOI: 10.11900/0412.1961.2025.00405

References

[1] Raabe D, Tasan C C, Olivetti E A. Strategies for improving the sustainability of structural metals [J]. Nature, 2019, 575: 64
[2] Huang J Z, Han J C, Wu T, et al. Boosting hydrogen transfer during volmer reaction at oxides/metal nanocomposites for efficient alkaline hydrogen evolution [J]. ACS Energy Lett., 2019, 4: 3002
[3] Fu Q, Han J C, Wang X J, et al. 2D transition metal dichalcogenides: Design, modulation, and challenges in electrocatalysis [J]. Adv. Mater., 2021, 33: 1907818
[4] Huang J Z, Sheng H Y, Ross R D, et al. Modifying redox properties and local bonding of Co3O4 by CeO2 enhances oxygen evolution catalysis in acid [J]. Nat. Commun., 2021, 12: 3036
[5] Yeh J W, Chen S K, Lin S J, et al. Nanostructured high-entropy alloys with multiple principal elements: Novel alloy design concepts and outcomes [J]. Adv. Eng. Mater., 2004, 6: 299
[6] Yeh J W. Alloy design strategies and future trends in high-entropy alloys [J]. JOM, 2013, 65: 1759
[7] Yeh J W. Physical metallurgy of high-entropy alloys [J]. JOM, 2015, 67: 2254
[8] Hsu W L, Tsai C W, Yeh A C, et al. Clarifying the four core effects of high-entropy materials [J]. Nat. Rev. Chem., 2024, 8: 471
[9] Sarkar A, Breitung B, Hahn H. High entropy oxides: The role of entropy, enthalpy and synergy [J]. Scr. Mater., 2020, 187: 43
[10] Csanádi T, Castle E, Reece M J, et al. Strength enhancement and slip behaviour of high-entropy carbide grains during micro-compression [J]. Sci. Rep., 2019, 9: 10200
[11] Qin M D, Yan Q Z, Wang H R, et al. High-entropy monoborides: Towards superhard materials [J]. Scr. Mater., 2020, 189: 101
[12] Wang R, Huang J Z, Zhang X H, et al. Two-dimensional high-entropy metal phosphorus trichalcogenides for enhanced hydrogen evolution reaction [J]. ACS Nano, 2022, 16: 3593
[13] Zhang Y, Li H, Liu X, et al. Sub-3 nm high-entropy alloy nanoparticles with triple functionalities for efficient electrolytic hydrogen production [J]. Adv. Mater., 2025, 37: e08975
[14] Yan S X, Luo S H, Yang L, et al. Novel P2-type layered medium-entropy ceramics oxide as cathode material for sodium-ion batteries [J]. J. Adv. Ceram., 2022, 11: 158
[15] Wyatt B C, Yang Y N, Micha?owski P P, et al. Order-to-disorder transition due to entropy in layered and 2D carbides [J]. Science, 2025, 389: 1054
[16] Zhang Q B, Gallant M C, Chen Y, et al. Isothermal solidification for high-entropy alloy synthesis [J]. Nature, 2025, 646: 323
[17] Sohail Y, Zhang C L, Xue D Z, et al. Machine-learning design of ductile FeNiCoAlTa alloys with high strength [J]. Nature, 2025, 643: 119
[18] Han X D, An Z B, Mao S C, et al. Negative mixing enthalpy alloying to promote the development of alloys with high strength and ductility [J]. Acta Metall. Sin., 2025, 61: 953
  韩晓东, 安子冰, 毛圣成 等. 负混合焓合金化推动高强韧合金发展 [J]. 金属学报, 2025, 61: 953
[19] Ma E, Liu C. Achieving alloys with concurrent high strength and high ductility [J]. Acta Metall. Sin., 2025, 61: 665
  马 恩, 刘 畅. 如何使合金兼具高强度与高塑性 [J]. 金属学报, 2025, 61: 665
[20] Zhong Y B, Shi P J. Hierarchical lamellar heterostructure design renders metallic materials with ultrahigh strength-ductility combinations [J]. Acta Metall. Sin., 2025, 61: 1593
  钟云波, 时培建. 多级层片异构设计构筑超高强塑性金属材料 [J]. 金属学报, 2025, 61: 1593
[21] Wang X Y, Liu Q D, Wang X. High-entropy materials: From bulk to sub-nano [J]. Adv. Funct. Mater., 2025, 35: 2504275
[22] Zhao P C, Cao Q G, Yi W, et al. Facile and general method to synthesize Pt-based high-entropy-alloy nanoparticles [J]. ACS Nano, 2022, 16: 14017
[23] Minamihara H, Kusada K, Wu D S, et al. Continuous-flow reactor synthesis for homogeneous 1 nm-sized extremely small high-entropy alloy nanoparticles [J]. J. Am. Chem. Soc., 2022, 144: 11525
[24] Wang S Q, Xu B L, Huo W Y, et al. Efficient FeCoNiCuPd thin-film electrocatalyst for alkaline oxygen and hydrogen evolution reactions [J]. Appl. Catal., 2022, 313B: 121472
[25] Cui Y F, Jiang S D, Fu Q, et al. Cost-effective high entropy core-shell fiber for stable oxygen evolution reaction at 2 A cm-2 [J]. Adv. Funct. Mater., 2023, 33: 2306889
[26] Ma Z B, Gao Y X, Ma C L, et al. A novel strategy for preparing high-entropy ceramics through full glass crystallization [J]. Energy Environ. Mater., 2025, 8: e70065
[27] Harrington T J, Gild J, Sarker P, et al. Phase stability and mechanical properties of novel high entropy transition metal carbides [J]. Acta Mater., 2019, 166: 271
[28] Sarker P, Harrington T, Toher C, et al. High-entropy high-hardness metal carbides discovered by entropy descriptors [J]. Nat. Commun., 2018, 9: 4980
[29] Wei X F, Liu J X, Li F, et al. High entropy carbide ceramics from different starting materials [J]. J. Eur. Ceram. Soc., 2019, 39: 2989
[30] Fu Z Z, Koc R. Pressureless sintering of submicron titanium carbide powders [J]. Ceram. Int., 2017, 43: 17233
[31] Chen L, Zhang W, Tan Y Q, et al. Influence of vanadium content on the microstructural evolution and mechanical properties of (TiZrHfVNbTa)C high-entropy carbides processed by pressureless sintering [J]. J. Eur. Ceram. Soc., 2021, 41: 60
[32] Gusm?o R, Sofer Z, Pumera M. Metal phosphorous trichalcogenides (MPCh3): From synthesis to contemporary energy challenges [J]. Angew. Chem. Int. Ed., 2019, 58: 9326
[33] Song B, Li K, Yin Y, et al. Tuning mixed nickel iron phosphosulfide nanosheet electrocatalysts for enhanced hydrogen and oxygen evolution [J]. ACS Catal., 2017, 7: 8549
[34] Wang R, Chen M X, Han J C, et al. Entropy engineering on 2D metal phosphorus trichalcogenides for surface-enhanced Raman scattering [J]. Adv. Funct. Mater., 2024, 34: 2312322
[35] Sarkar A, Wang Q S, Schiele A, et al. High-entropy oxides: Fundamental aspects and electrochemical properties [J]. Adv. Mater., 2019, 31: 1806236
[36] Wu H, Lu Q, Li Y J, et al. Rapid Joule-heating synthesis for manufacturing high-entropy oxides as efficient electrocatalysts [J]. Nano Lett., 2022, 22: 6492
[37] Zhou W X, Tang Y J, Zhang X Y, et al. MOF derived metal oxide composites and their applications in energy storage [J]. Coord. Chem. Rev., 2023, 477: 214949
[38] Rafique M, Yao T T, Ma S Y, et al. High-entropy engineering of cobalt spinel oxide breaks the activity-stability trade-off in oxygen evolution reaction [J]. Adv. Funct. Mater., 2026, 36: e12495
[39] Kim E, Kim S, Kim Y, et al. Activation of hidden catalytic sites in 2D basal plane via p-n heterojunction interface engineering toward efficient oxygen evolution reaction [J]. Adv. Energy Mater., 2025, 15: 2403722
[40] Liu H Q, Xiong R, Yao T T, et al. Application and development of PEM water electrolysis technology in the aerospace field [J]. J. Zhengzhou Univ. Aeronaut., 2025, 43(4): 1
  刘恒岐, 熊 睿, 姚田田 等. PEM水电解技术在航天领域的应用与发展 [J]. 郑州航空工业管理学院学报, 2025, 43(4): 1
[41] Li B, Jiang S D, Fu Q, et al. Tailoring nanocrystalline/amorphous interfaces to enhance oxygen evolution reaction performance for FeNi-based alloy fibers [J]. Adv. Funct. Mater., 2025, 35: 2413088
Outlines

/