AI Chat Paper
Discover the SciOpen Platform and Achieve Your Research Goals with Ease.
Dense monolithic (Ti,Zr,Hf)C/SiC ceramic nanocomposites with four different molar ratios of metallic elements in the (Ti,Zr,Hf)C phase (i.e., Ti : Zr : Hf = 1 : 1 : 1, 2 : 3 : 5, 2 : 3 : 3, and 1 : 2 : 1) were prepared upon pyrolysis of novel (Ti,Zr,Hf)-containing single-source precursors (SSPs), followed by spark plasma sintering (SPS). A thorough characterization was conducted to elucidate the synthesis of the SSPs, polymer-to-ceramic transformation, chemical/phase compositions, and microstructure of the SiTiZrHfC-based ceramics. The results revealed the feasibility of synthesizing nanocomposites with high (Ti,Zr,Hf)C contents using the SSP method. These nanocomposites were characterized by a unique microstructure with in situ generated (Ti,Zr,Hf)C@C core–shell nanoparticles homogeneously mixed with β-SiC. The ablation behavior of the nanocomposites was evaluated on an air-plasma device for 60 s. Impressively, the nanocomposites exhibited excellent ablation resistance, and the lowest linear ablation rate reached −0.58 μm/s at 2200 °C. Notably, the ablation resistance can be dramatically improved by precisely tailoring the atomic ratios of metal elements within the (Ti,Zr,Hf)C phase via the molecular design of the SSPs. The formation of a multiple-oxide layer with both a high-melting-point phase ((Ti,Zr,Hf)O2) and low-melting-point phases ((Zr,Hf)TiO4) and glassy SiO2, as well as their structure, played a critical role in the enhanced ablation resistance. The uniform distribution of the high-melting-point (Ti,Zr,Hf)O2 nano/microparticles throughout the glassy SiO2 matrix significantly enhanced the viscosity and stability of the oxide layer by the pinning effect, offering superior protection against the ingress of oxygen atoms and excellent resistance to mechanical erosion.
Zeng Y, Wang DN, Xiong X, et al. Ablation-resistant carbide Zr0.8Ti0.2C0.74B0.26 for oxidizing environments up to 3 000 °C. Nat Commun 2017, 8: 15836.
Zhang YY, Sun J, Guo LX, et al. Ablation resistant ZrC coating modified by polymer-derived SiC/TiC nanocomposites for ultra-high temperature application. J Eur Ceram Soc 2022, 42: 18–29.
Ye BL, Wen TQ, Nguyen MC, et al. First-principles study, fabrication and characterization of (Zr0.25Nb0.25Ti0.25V0.25)C high-entropy ceramics. Acta Mater 2019, 170: 15–23.
Ni DW, Cheng Y, Zhang JP, et al. Advances in ultra-high temperature ceramics, composites, and coatings. J Adv Ceram 2022, 11: 1–56.
Zhang J, Zhang YL, Fu YQ, et al. Preparation and ablation behavior of HfC–SiC co-deposited coatings with different proportions. Corros Sci 2021, 192: 109853.
Shi AH, Yang X, Fang CQ, et al. Mechanical and ablative properties improvement of HfC–SiC coatings upon introduction of TiC. J Eur Ceram Soc 2022, 42: 4735–4747.
Jiao XY, Tan Q, He QC, et al. Cyclic ablation behavior of mullite-modified C/C–HfC–SiC composites under an oxyacetylene flame at about 2400 °C. J Eur Ceram Soc 2023, 43: 4309–4321.
Harrington TJ, Gild J, Sarker P, et al. Phase stability and mechanical properties of novel high entropy transition metal carbides. Acta Mater 2019, 166: 271–280.
Chen L, Zhang W, Lu WY, et al. Low thermal conductivity of dense (TiZrHfVNbTa)C x high-entropy carbides by tailoring carbon stoichiometry. J Adv Ceram 2023, 12: 49–58.
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: 1082–1092.
Lun HL, Zeng Y, Xiong X, et al. Oxidation behavior of non-stoichiometric (Zr,Hf,Ti)C x carbide solid solution powders in air. J Adv Ceram 2021, 10: 741–757.
Wang YC, Zhang BH, Zhang CY, et al. Ablation behaviour of (Hf–Ta–Zr–Nb)C high entropy carbide ceramic at temperatures above 2100 °C. J Mater Sci Technol 2022, 113: 40–47.
Zhou JY, Zhang JY, Zhang F, et al. High-entropy carbide: A novel class of multicomponent ceramics. Ceram Int 2018, 44: 22014–22018.
Li JC, Zhang YL, Lv JS, et al. Sealing role of Ti-rich phase in HfC–ZrC–TiC coating for C/C composites during ablation above 2100 °C. Corros Sci 2022, 205: 110474.
Bargeron CB, Benson RC, Jette AN, et al. Oxidation of hafnium carbide in the temperature range 1400° to 2060 °C. J Am Ceram Soc 1993, 76: 1040–1046.
Backman L, Opila EJ. Thermodynamic assessment of the group IV, V and VI oxides for the design of oxidation resistant multi-principal component materials. J Eur Ceram Soc 2019, 39: 1796–1802.
Pan XH, Niu YR, Xu XT, et al. Long time ablation behaviors of designed ZrC–SiC–TiC ternary coatings for environments above 2000 °C. Corros Sci 2020, 170: 108645.
Pan XH, Niu YR, Liu T, et al. Ablation behaviors of ZrC-TiC coatings prepared by vacuum plasma spray: Above 2000 °C. J Eur Ceram Soc 2019, 39: 3292–3300.
Ye ZM, Zeng Y, Xiong X, et al. Elucidating the role of preferential oxidation during ablation: Insights on the design and optimization of multicomponent ultra-high temperature ceramics. J Adv Ceram 2022, 11: 1956–1975.
Wang YC, Yu D, Yin J, et al. Ablation behavior of (Hf–Ta–Zr–Nb–Ti)C high-entropy carbide and (Hf–Ta–Zr–Nb–Ti)C– xSiC composites. J Am Ceram Soc 2022, 105: 6395–6406.
Gong ZY, Zhao W, Guan K, et al. Influence of grain boundary and grain size on the mechanical properties of polycrystalline ceramics: Grain-scale simulations. J Am Ceram Soc 2020, 103: 5900–5913.
Ionescu E, Linck C, Fasel C, et al. Polymer-derived SiOC/ZrO2 ceramic nanocomposites with excellent high-temperature stability. J Am Ceram Soc 2010, 93: 241–250.
Wen QB, Xu YP, Xu BB, et al. Single-source-precursor synthesis of dense SiC/HfC x N1– x -based ultrahigh-temperature ceramic nanocomposites. Nanoscale 2014, 6: 13678–13689.
Wen QB, Yu ZJ, Xu YP, et al. SiC/Hf y Ta1– y C x N1– x /C ceramic nanocomposites with Hf y Ta1– y C x N1– x –carbon core–shell nanostructure and the influence of the carbon-shell thickness on electrical properties. J Mater Chem C 2018, 6: 855–864.
Qian BJ, Cao BW, Chu MY, et al. Curing reactions of liquid hydridopolycarbosilanes with vinyl or allyl groups. J Appl Polym Sci 2023, 140: 54565.
Li KJ, Li SG, Li N, et al. Tetrakis(dimethylamido)hafnium adsorption and reaction on hydrogen terminated Si(100) surfaces. J Phys Chem C 2010, 114: 14061–14075.
Wen QB, Yu ZJ, Liu XM, et al. Mechanical properties and electromagnetic shielding performance of single-source-precursor synthesized dense monolithic SiC/HfC x N1– x /C ceramic nanocomposites. J Mater Chem C 2019, 7: 10683–10693.
Yang JC, Wen QB, Feng B, et al. Microstructural evolution and electromagnetic wave absorbing performance of single-source-precursor-synthesized SiCuCN-based ceramic nanocomposites. J Adv Ceram 2023, 12: 1299–1316.
Feng B, Peter J, Fasel C, et al. High-temperature phase and microstructure evolution of polymer-derived SiZrCN and SiZrBCN ceramic nanocomposites. J Am Ceram Soc 2020, 103: 7001–7013.
Yuan J, Hapis S, Breitzke H, et al. Single-source-precursor synthesis of hafnium-containing ultrahigh-temperature ceramic nanocomposites (UHTC–NCs). Inorg Chem 2014, 53: 10443–10455.
Yu ZJ, Li F, Zhu QK. Single-source-precursor synthesis and phase evolution of NbC–SiC–C ceramic nanocomposites with core–shell structured NbC@C and SiC@C nanoparticles. Adv Powder Mater 2022, 1: 100009.
Yu ZJ, Yang YJ, Mao KW, et al. Single-source-precursor synthesis and phase evolution of SiC–TaC–C ceramic nanocomposites containing core–shell structured TaC@C nanoparticles. J Adv Ceram 2020, 9: 320–328.
Lu L, Wen TH, Li W, et al. Single-source-precursor synthesis of dense monolithic SiC/(Ti0.25Zr0.25Hf0.25Ta0.25)C ceramic nanocomposite with excellent high-temperature oxidation resistance. J Eur Ceram Soc 2024, 44: 595–609.
Rodríguez-Carvajal J. Recent advances in magnetic structure determination by neutron powder diffraction. Physica B 1993, 192: 55–69.
Li WJ, Li D, Gao X, et al. A study on the thermal conversion of scheelite-type ABO4 into perovskite-type AB(O,N)3. Dalton T 2015, 44: 8238–8246.
Holzwarth U, Gibson N. The Scherrer equation versus the ‘Debye–Scherrer equation’. Nat Nanotechnol 2011, 6: 534.
Wen QB, Yu ZJ, Riedel R. The fate and role of in situ formed carbon in polymer-derived ceramics. Prog Mater Sci 2020, 109: 100623.
Nemanich RJ, Solin SA. First- and second-order Raman scattering from finite-size crystals of graphite. Phys Rev B 1979, 20: 392–401.
Nakashima S, Harima H. Raman investigation of SiC polytypes. 3.0.CO;2-L">Phys Status Solidi A 1997, 162: 39–64.
Mera G, Navrotsky A, Sen S, et al. Polymer-derived SiCN and SiOC ceramics–Structure and energetics at the nanoscale. J Mater Chem A 2013, 1: 3826–3836.
Wen QB, Feng Y, Yu ZJ, et al. Microwave absorption of SiC/HfC x N1– x /C ceramic nanocomposites with HfC x N1– x –carbon core–shell particles. J Am Ceram Soc 2016, 99: 2655–2663.
Zhang XH, Du BH, Hu P, et al. Thermal response, oxidation and ablation of ultra-high temperature ceramics, C/SiC, C/C, graphite and graphite–ceramics. J Mater Sci Technol 2022, 102: 137–158.
Zhang XX, Yang X, Luo X, et al. Formation mechanism of (Ti,Zr,Hf)C medium-entropy carbide derived from polymer precursors and its modification on the ablative mechanism of C/C–SiC composites. Corros Sci 2024, 230: 111935.
Feng GH, Li HJ, Yao XY, et al. Evaluation of ablation resistant ZrC–SiC multilayer coating for SiC coated carbon/carbon composites under oxyacetylene and laser conditions. Corros Sci 2022, 205: 110427.
Xiang LY, Cheng LF, Fan XM, et al. Effect of interlayer on the ablation properties of laminated HfC–SiC ceramics under oxyacetylene torch. Corros Sci 2015, 93: 172–179.
Peng Z, Sun W, Xiong X, et al. Novel refractory high-entropy ceramics: Transition metal carbonitrides with superior ablation resistance. Corros Sci 2021, 184: 109359.
Zhang J, Jiang JM, Song Q, et al. Ultra-high temperature ablation property of Ta0.5Hf0.5C ternary ceramic under plasma flame. Ceram Int 2021, 47: 28050–28054.
Guo WJ, Hu J, Ye YC, et al. Ablation behavior of (TiZrHfNbTa)C high-entropy ceramics with the addition of SiC secondary under an oxyacetylene flame. Ceram Int 2022, 48: 12790–12799.
Ni N, Ding Q, Shi YC, et al. Ablation behavior of high-entropy carbides ceramics (Hf0.2Zr0.2Ta0.2Nb0.2Ti0.2)C upon exposition to an oxyacetylene torch at 2000 °C. J Eur Ceram Soc 2023, 43: 2306–2319.
Bourova E, Richet P. Quartz and cristobalite: High-temperature cell parameters and volumes of fusion. Geophys Res Lett 1998, 25: 2333–2336.
Coutures JP, Coutures J. The system HfO2–TiO2. J Am Ceram Soc 1987, 70: 383–387.
Shen YZ, Sun W, Xu YL, et al. Structural characteristics and ablative behavior of YF3 modified C/C–ZrC–SiC composites and their preparation by molten salt assisted reactive melt infiltration. J Eur Ceram Soc 2023, 43: 1303–1314.
Castle E, Csanádi T, Grasso S, et al. Processing and properties of high-entropy ultra-high temperature carbides. Sci Rep 2018, 8: 8609.
Cai FY, Ni DW, Bao WC, et al. Ablation behavior and mechanisms of Cf/(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)C–SiC high-entropy ceramic matrix composites. Compos Part B Eng 2022, 243: 110177.
Cai FY, Ni DW, Chen BW, et al. Fabrication and properties of Cf/(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)C–SiC high-entropy ceramic matrix composites via precursor infiltration and pyrolysis. J Eur Ceram Soc 2021, 41: 5863–5871.
Cui YY, Li AJ, Li B, et al. Microstructure and ablation mechanism of C/C–SiC composites. J Eur Ceram Soc 2014, 34: 171–177.
Berton B, Bacos MP, Demange D, et al. High-temperature oxidation of silicon carbide in simulated atmospheric re-entry conditions. J Mater Sci 1992, 27: 3206–3210.
Jing X, Zhao W, Lan L. The effect of particle size on electric conducting percolation threshold in polymer/conducting particle composites. J Mater Sci Lett 2000, 19: 377–379.
Li H, Zhang LT, Zeng QF, et al. Thermodynamic calculation of HfB2 volatility diagram. J Phase Equilib Diff 2011, 32: 422–427.
Zou J, Rubio V, Binner J. Thermoablative resistance of ZrB2–SiC–WC ceramics at 2400 °C. Acta Mater 2017, 133: 293–302.
Wang DN, Zeng Y, Xiong X, et al. Ablation behavior of ZrB2–SiC protective coating for carbon/carbon composites. Ceram Int 2015, 41: 7677–7686.
Kusano E. Homologous substrate-temperature dependence of structure and properties of TiO2, ZrO2, and HfO2 thin films deposited by reactive sputtering. J Vac Sci Technol A 2019, 37: 051508.
Zhang JP, Hou JQ, Zhou L, et al. TaSi2-modified HfB2–SiC coating: Preparation and ablation behavior. J Am Ceram Soc 2024, 107: 461–474.
Jayaseelan DD, Zapata-Solvas E, Chater RJ, et al. Structural and compositional analyses of oxidised layers of ZrB2-based UHTCs. J Eur Ceram Soc 2015, 35: 4059–4071.
Li C, Niu YR, Liu T, et al. Effect of WB on oxidation behavior and microstructure evolution of ZrB2–SiC coating. Corros Sci 2019, 155: 155–163.
584
Views
185
Downloads
0
Crossref
0
Web of Science
0
Scopus
0
CSCD
Altmetrics
This is an open access article under the terms of the Creative Commons Attribution 4.0 International License (CC BY 4.0, http://creativecommons.org/licenses/by/4.0/).
