AI Chat Paper
Note: Please note that the following content is generated by AMiner AI. SciOpen does not take any responsibility related to this content.
{{lang === 'zh_CN' ? '文章概述' : 'Summary'}}
{{lang === 'en_US' ? '中' : 'Eng'}}
Chat more with AI
PDF (1.6 MB)
Collect
Submit Manuscript AI Chat Paper
Show Outline
Outline
Show full outline
Hide outline
Outline
Show full outline
Hide outline
Research Article | Open Access

Fabrication of multi-anionic high-entropy carbonitride ultra-high-temperature ceramics by a green and low-cost process with excellent mechanical properties

Liansen XiaaShun Donga( )Jianqiang XinbKaixuan GuicPeitao HuaYongshuai XieaDongdong YangaXinghong ZhangaYanchun Zhoud( )
National Key Laboratory of Science and Technology on Advanced Composites in Special Environments, Harbin Institute of Technology, Harbin 150001, China
Institute for Aero Engine, Tsinghua University, Beijing 100084, China
School of Materials Science and Engineering, Anhui Polytechnic University, Wuhu 241000, China
School of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450001, China
Show Author Information

Graphical Abstract

Abstract

As a new category of ultra-high-temperature ceramics (UHTCs), multi-anionic high-entropy (HE) carbonitride UHTCs are expected to have better comprehensive performance than conventional UHTCs. However, how to realize the green and low-cost synthesis of high-quality multi-anionic HE carbonitride UHTC powders and prepare bulk ceramics with excellent mechanical properties still faces great challenges. In this work, a green, low-cost, and controllable preparation process of (Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)CxN1−x powders is achieved by sol–gel combined with the carbothermal reduction/nitridation method for the first time. The as-synthesized (Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)CxN1−x powders possess high compositional uniformity and controllable particle size. In addition, the obtained bulk ceramics prepared at 1800 ℃ exhibit superior fracture toughness (KIC) of 5.39± 0.16 MPa·m1/2 and high nanohardness of 35.75±1.23 GPa, elastic modulus (E) of 566.70±8.68 GPa, and flexural strength of 487±41 MPa. This study provides a feasible strategy for preparing the high-performance HE carbonitride ceramics in a more environmentally friendly and economical manner.

References

[1]
Xiang HM, Xing Y, Dai FZ, et al. High-entropy ceramics: Present status, challenges, and a look forward. J Adv Ceram 2021, 10: 385441.
[2]
Akrami S, Edalati P, Fuji M, et al. High-entropy ceramics: Review of principles, production and applications. Mater Sci Eng R 2021, 146: 100644.
[3]
Gu JF, Zou J, Sun SK, et al. Dense and pure high-entropy metal diboride ceramics sintered from self-synthesized powders via boro/carbothermal reduction approach. Sci China Mater 2019, 62: 18981909.
[4]
Ni DW, Cheng Y, Zhang JP, et al. Advances in ultra-high temperature ceramics, composites, and coatings. J Adv Ceram 2022, 11: 156.
[5]
Castle E, Csanádi T, Grasso S, et al. Processing and properties of high-entropy ultra-high temperature carbides. Sci Rep 2018, 8: 8609.
[6]
Wang K, Chen L, Xu CG, et al. Microstructure and mechanical properties of (TiZrNbTaMo)C high-entropy ceramic. J Mater Sci Technol 2020, 39: 99105.
[7]
Wang YC, Reece MJ. Oxidation resistance of (Hf–Ta–Zr–Nb)C high entropy carbide powders compared with the component monocarbides and binary carbide powders. Scripta Mater 2021, 193: 8690.
[8]
Lun HL, Zeng Y, Xiong X, et al. Oxidation behavior of non-stoichiometric (Zr,Hf,Ti)Cx carbide solid solution powders in air. J Adv Ceram 2021, 10: 741757.
[9]
Chen H, Xiang HM, Dai FZ, et al. High porosity and low thermal conductivity high entropy (Zr0.2Hf0.2Ti0.2Nb0.2Ta0.2)C. J Mater Sci Technol 2019, 35: 17001705.
[10]
Yan XL, Constantin L, Lu YF, et al. (Hf0.2Zr0.2Ta0.2Nb0.2Ti0.2)C high-entropy ceramics with low thermal conductivity. J Am Ceram Soc 2018, 101: 44864491.
[11]
Shao ZJ, Wu Z, Sun LC, et al. High entropy ultra-high temperature ceramic thermal insulator (Zr1/5Hf1/5Nb1/5 Ta1/5Ti1/5)C with controlled microstructure and outstanding properties. J Mater Sci Technol 2022, 119: 190199.
[12]
Song JT, Chen GQ, Xiang HM, et al. Regulating the formation ability and mechanical properties of high-entropy transition metal carbides by carbon stoichiometry. J Mater Sci Technol 2022, 121: 181189.
[13]
Qin Y, Liu JX, Liang YC, et al. Equiatomic 9-cation high-entropy carbide ceramics of the IVB, VB, and VIB groups and thermodynamic analysis of the sintering process. J Adv Ceram 2022, 11: 10821092.
[14]
Chen L, Zhang W, Tan YQ, et al. Influence of vanadium content on the microstructural evolution and mechanical properties of (TiZrHfVNbTa)C high-entropy carbides processed by pressureless sintering. J Eur Ceram Soc 2021, 41: 6067.
[15]
Luo SC, Guo WM, Fang ZL, et al. Effect of carbon content on the microstructure and mechanical properties of high-entropy (Ti0.2Zr0.2Nb0.2Ta0.2Mo0.2)Cx ceramics. J Eur Ceram Soc 2022, 42: 336343.
[16]
Zhang Y, Sun SK, Guo WM, et al. Optimal preparation of high-entropy boride-silicon carbide ceramics. J Adv Ceram 2021, 10: 173180.
[17]
Guo RR, Li ZJ, Li L, et al. Microstructures and oxidation mechanisms of (Zr0.2Hf0.2Ta0.2Nb0.2Ti0.2)B2 high-entropy ceramic. J Eur Ceram Soc 2022, 42: 21272134.
[18]
Moskovskikh D, Vorotilo S, Buinevich V, et al. Extremely hard and tough high entropy nitride ceramics. Sci Rep 2020, 10: 19874.
[19]
Jin T, Sang XH, Unocic RR, et al. Mechanochemical-assisted synthesis of high-entropy metal nitride via a soft urea strategy. Adv Mater 2018, 30: 1707512.
[20]
Kretschmer A, Holec D, Yalamanchili K, et al. Strain-stabilized Al-containing high-entropy sublattice nitrides. Acta Mater 2022, 224: 117483.
[21]
Qin Y, Liu JX, Li F, et al. A high entropy silicide by reactive spark plasma sintering. J Adv Ceram 2019, 8: 148152.
[22]
Liu L, Zhang LQ, Liu D. Complete elimination of pest oxidation by high entropy refractory metallic silicide (Mo0.2W0.2Cr0.2Ta0.2Nb0.2)Si2. Scripta Mater 2020, 189: 2529.
[23]
Gild J, Braun J, Kaufmann K, et al. A high-entropy silicide: (Mo0.2Nb0.2Ta0.2Ti0.2W0.2)Si2. J Materiomics 2019, 5: 337343.
[24]
Song JT, Cheng Y, Xiang HM, et al. Medium and high-entropy transition mental disilicides with improved infrared emissivity for thermal protection applications. J Mater Sci Technol 2023, 136: 149158.
[25]
Zhang P, Liu XJ, Cai AH, et al. High-entropy carbide–nitrides with enhanced toughness and sinterability. Sci China Mater 2021, 64: 20372044.
[26]
Wen TQ, Ye BL, Nguyen MC, et al. Thermophysical and mechanical properties of novel high-entropy metal nitride-carbides. J Am Ceram Soc 2020, 103: 64756489.
[27]
Dippo OF, Mesgarzadeh N, Harrington TJ, et al. Bulk high-entropy nitrides and carbonitrides. Sci Rep 2020, 10: 21288.
[28]
Han XQ, Lin N, Li AQ, et al. Microstructure and characterization of (Ti,V,Nb,Ta)(C,N) high-entropy ceramic. Ceram Int 2021, 47: 3510535110.
[29]
Jing C, Zhou SJ, Zhang W, et al. Low temperature synthesis and densification of (Ti,V,Nb,Ta,Mo)(C,N) high-entropy carbonitride ceramics. J Alloys Compd 2022, 927: 167095.
[30]
Li F, Lu Y, Wang XG, et al. Liquid precursor-derived high-entropy carbide nanopowders. Ceram Int 2019, 45: 2243722441.
[31]
Du B, Huang XM, Wang AZ, et al. Structure evolutions of the polymer derived medium-/high-entropy metal carbides. J Alloys Compd 2023, 939: 168737.
[32]
Sun YN, Chen FH, Qiu WF, et al. Synthesis of rare earth containing single-phase multicomponent metal carbides via liquid polymer precursor route. J Am Ceram Soc 2020, 103: 60816087.
[33]
Song JT, Han WB, Dong S, et al. Constructing hydrothermal carbonization coatings on carbon fibers with controllable thickness for achieving tunable sorption of dyes and oils via a simple heat-treated route. J Colloid Interf Sci 2020, 559: 263272.
[34]
Fang C, Hu P, Dong S, et al. An efficient hydrothermal transformation approach for construction of controllable carbon coating on carbon fiber from renewable carbohydrate. Appl Surf Sci 2019, 491: 478487.
[35]
Li F, Huang X, Liu JX, et al. Sol–gel derived porous ultra-high temperature ceramics. J Adv Ceram 2020, 9: 116.
[36]
Sun BQ, Chen DM, Cheng Y, et al. Sugar-derived isotropic nanoscale polycrystalline graphite capable of considerable plastic deformation. Adv Mater 2022, 34: 2200363.
[37]
Gasparrini C, Rana DS, Le Brun N, et al. On the stoichiometry of zirconium carbide. Sci Rep 2020, 10: 6347.
[38]
Niihara K, Morena R, Hasselman DPH. Evaluation of KIC of brittle solids by the indentation method with low crack-to-indent ratios. J Mater Sci Lett 1982, 1: 1316.
[39]
Feng L, Fahrenholtz WG, Hilmas GE, et al. Synthesis of single-phase high-entropy carbide powders. Scripta Mater 2019, 162: 9093.
[40]
Peng C, Gao X, Wang MZ, et al. Diffusion-controlled alloying of single-phase multi-principal transition metal carbides with high toughness and low thermal diffusivity. Appl Phys Lett 2019, 114: 011905.
[41]
Vasanthakumar K, Revathi G, Ariharan S, et al. Novel single phase (Ti0.2W0.2Ta0.2Mo0.2V0.2)C0.8 high entropy carbide using ball milling followed by reactive spark plasma sintering. J Eur Ceram Soc 2021, 41: 67566762.
[42]
Sarkar A, Djenadic R, Wang D, et al. Rare earth and transition metal based entropy stabilised perovskite type oxides. J Eur Ceram Soc 2018, 38: 23182327.
[43]
Peng B, Zhang H, Shao HZ, et al. Low lattice thermal conductivity of stanene. Sci Rep 2016, 6: 20225.
[44]
Yang Y, Ma L, Gan GY, et al. Investigation of thermodynamic properties of high entropy (TaNbHfTiZr)C and (TaNbHfTiZr)N. J Alloys Compd 2019, 788: 10761083.
[45]
Jiang DY. Recent progresses in the phenomenological description for the indentation size effect in microhardness testing of brittle ceramics. J Adv Ceram 2012, 1: 3849.
[46]
Niihara K. A fracture mechanics analysis of indentation-induced Palmqvist crack in ceramics. J Mater Sci Lett 1983, 2: 221223.
[47]
Liu DQ, Zhang AJ, Jia JG, et al. Reaction synthesis and characterization of a new class high entropy carbide (NbTaMoW)C. Mater Sci Eng A 2021, 804: 140520.
[48]
Lu K, Liu JX, Wei XF, et al. Microstructures and mechanical properties of high-entropy (Ti0.2Zr0.2Hf0.2Nb0.2 Ta0.2)C ceramics with the addition of SiC secondary phase. J Eur Ceram Soc 2020, 40: 18391847.
[49]
Feng L, Chen WT, Fahrenholtz WG, et al. Strength of single-phase high-entropy carbide ceramics up to 2300 ℃. J Am Ceram Soc 2021, 104: 419427.
[50]
Sun KB, Yang ZW, Mu RJ, et al. Densification and joining of a (HfTaZrNbTi)C high-entropy ceramic by hot pressing. J Eur Ceram Soc 2021, 41: 31963206.
[51]
Liu DQ, Zhang AJ, Jia JG, et al. Phase evolution and properties of (VNbTaMoW)C high entropy carbide prepared by reaction synthesis. J Eur Ceram Soc 2020, 40: 27462751.
[52]
Zhang W, Chen L, Lu WY, et al. Non-stoichiometry of (TiZrHfVNbTa)Cx and its significance to the microstructure and mechanical properties. J Eur Ceram Soc 2022, 42: 63476355.
[53]
Yu D, Yin J, Zhang BH, et al. Pressureless sintering and properties of (Hf0.2Zr0.2Ta0.2Nb0.2Ti0.2)C high-entropy ceramics: The effect of pyrolytic carbon. J Eur Ceram Soc 2021, 41: 38233831.
[54]
Demirskyi D, Borodianska H, Suzuki TS, et al. High-temperature flexural strength performance of ternary high-entropy carbide consolidated via spark plasma sintering of TaC, ZrC and NbC. Scripta Mater 2019, 164: 1216.
[55]
Kondo S, Mitsuma T, Shibata N, et al. Direct observation of individual dislocation interaction processes with grain boundaries. Sci Adv 2016, 2: 1501926.
[56]
Li R, Luo RY, Lin N, et al. A novel strategy for fabricating (Ti,Ta,Nb,Zr,W)(C,N) high-entropy ceramic reinforced with in situ synthesized W2C particles. Ceram Int 2022, 48: 3254032545.
[57]
Boccaccini AR. Machinability and brittleness of glass-ceramics. J Mater Process Tech 1997, 65: 302304.
Journal of Advanced Ceramics
Pages 1258-1272
Cite this article:
Xia L, Dong S, Xin J, et al. Fabrication of multi-anionic high-entropy carbonitride ultra-high-temperature ceramics by a green and low-cost process with excellent mechanical properties. Journal of Advanced Ceramics, 2023, 12(6): 1258-1272. https://doi.org/10.26599/JAC.2023.9220755

3002

Views

787

Downloads

15

Crossref

12

Web of Science

13

Scopus

2

CSCD

Altmetrics

Received: 01 February 2023
Revised: 14 April 2023
Accepted: 16 April 2023
Published: 29 May 2023
© The Author(s) 2023.

Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if changes were made.

The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder.

To view a copy of this licence, visit http://creativecommons.org/licenses/by/4.0/.

Return