Journal Home > Volume 12 , Issue 7
Journal of Advanced Ceramics 2023, 12(7): 1418-1429 https://doi.org/10.26599/JAC.2023.9220764
Research Article | Open Access | Issue | Published: 06 July 2023

Hard and tough novel high-pressure γ-Si3N4/Hf3N4 ceramic nanocomposites

Show Author's Information Wei Lia,  Zhaoju Yub( ),  Leonore Wiehla,  Tianshu Jianga,  Ying Zhana,  Emmanuel III Ricohermosoa,  Martin Etterc,  Emanuel Ionescua,d,  Qingbo Wene,  Christian Lathec,f,  Robert Farlac,  Dharma Teppala Tejaa,  Sebastian Brunsa,  Marc Widenmeyera,  Anke Weidenkaffa,d,  Leopoldo Molina-Lunaa,  Ralf Riedela,  Shrikant Bhatc
Department of Materials and Earth Sciences, Technical University of Darmstadt, Darmstadt 64283, Germany
Key Laboratory of High Performance Ceramic Fibers (Xiamen University), Ministry of Education, College of Materials, Xiamen University, Xiamen 361005, China
Deutsches Elektronen-Synchrotron DESY, Hamburg 22607, Germany
Fraunhofer IWKS, Department Digitalization of Resources, Alzenau 63755, Germany
State Key Laboratory of Powder Metallurgy, Central South University, Changsha 410083, China
Deutsches GeoForschungsZentrum Potsdam, Potsdam 14473, Germany
Keywords:
mechanical properties, thermal stability, ceramic nanocomposites, cubic silicon nitride (γ-Si3N4)/Hf3N4, in situ synchrotron radiation
Cite this article:
Li W, Yu Z, Wiehl L, et al. Hard and tough novel high-pressure γ-Si3N4/Hf3N4 ceramic nanocomposites. Journal of Advanced Ceramics, 2023, 12(7): 1418-1429. https://doi.org/10.26599/JAC.2023.9220764
Download citation
EndNote(RIS)
BibTeX

2195

Views

313

Downloads

Citations

2

Crossref

1

WoS

1

Scopus

0

CSCD

Abstract Full text Electronic supplementary material About this article

Cubic silicon nitride (γ-Si3N4) is superhard and one of the hardest materials after diamond and cubic boron nitride (cBN), but has higher thermal stability in an oxidizing environment than diamond, making it a competitive candidate for technological applications in harsh conditions (e.g., drill head and abrasives). Here, we report the high-pressure synthesis and characterization of the structural and mechanical properties of a γ-Si3N4/Hf3N4 ceramic nanocomposite derived from single-phase amorphous silicon (Si)–hafnium (Hf)–nitrogen (N) precursor. The synthesis of the γ-Si3N4/Hf3N4 nanocomposite is performed at ~20 GPa and ca. 1500 ℃ in a large volume multi anvil press. The structural evolution of the amorphous precursor and its crystallization to γ-Si3N4/Hf3N4 nanocomposites under high pressures is assessed by the in situ synchrotron energy-dispersive X-ray diffraction (ED-XRD) measurements at ~19.5 GPa in the temperature range of ca. 1000–1900 ℃. The fracture toughness (KIC) of the two-phase nanocomposite amounts ~6/6.9 MPa·m1/2 and is about 2 times that of single-phase γ-Si3N4, while its hardness of ca. 30 GPa remains high. This work provides a reliable and feasible route for the synthesis of advanced hard and tough γ-Si3N4-based nanocomposites with excellent thermal stabililty.


menu
Abstract
Full text
Outline
Electronic supplementary material
About this article

Hard and tough novel high-pressure γ-Si3N4/Hf3N4 ceramic nanocomposites

Show Author's information Wei Lia, Zhaoju Yub( ), Leonore Wiehla, Tianshu Jianga, Ying Zhana, Emmanuel III Ricohermosoa, Martin Etterc, Emanuel Ionescua,d, Qingbo Wene, Christian Lathec,f, Robert Farlac, Dharma Teppala Tejaa, Sebastian Brunsa, Marc Widenmeyera, Anke Weidenkaffa,d, Leopoldo Molina-Lunaa, Ralf Riedela, Shrikant Bhatc
Department of Materials and Earth Sciences, Technical University of Darmstadt, Darmstadt 64283, Germany
Key Laboratory of High Performance Ceramic Fibers (Xiamen University), Ministry of Education, College of Materials, Xiamen University, Xiamen 361005, China
Deutsches Elektronen-Synchrotron DESY, Hamburg 22607, Germany
Fraunhofer IWKS, Department Digitalization of Resources, Alzenau 63755, Germany
State Key Laboratory of Powder Metallurgy, Central South University, Changsha 410083, China
Deutsches GeoForschungsZentrum Potsdam, Potsdam 14473, Germany

Abstract

Cubic silicon nitride (γ-Si3N4) is superhard and one of the hardest materials after diamond and cubic boron nitride (cBN), but has higher thermal stability in an oxidizing environment than diamond, making it a competitive candidate for technological applications in harsh conditions (e.g., drill head and abrasives). Here, we report the high-pressure synthesis and characterization of the structural and mechanical properties of a γ-Si3N4/Hf3N4 ceramic nanocomposite derived from single-phase amorphous silicon (Si)–hafnium (Hf)–nitrogen (N) precursor. The synthesis of the γ-Si3N4/Hf3N4 nanocomposite is performed at ~20 GPa and ca. 1500 ℃ in a large volume multi anvil press. The structural evolution of the amorphous precursor and its crystallization to γ-Si3N4/Hf3N4 nanocomposites under high pressures is assessed by the in situ synchrotron energy-dispersive X-ray diffraction (ED-XRD) measurements at ~19.5 GPa in the temperature range of ca. 1000–1900 ℃. The fracture toughness (KIC) of the two-phase nanocomposite amounts ~6/6.9 MPa·m1/2 and is about 2 times that of single-phase γ-Si3N4, while its hardness of ca. 30 GPa remains high. This work provides a reliable and feasible route for the synthesis of advanced hard and tough γ-Si3N4-based nanocomposites with excellent thermal stabililty.

Keywords: mechanical properties, thermal stability, ceramic nanocomposites, cubic silicon nitride (γ-Si3N4)/Hf3N4, in situ synchrotron radiation

References(66)

[1]
Zerr A, Miehe G, Serghiou G, et al. Synthesis of cubic silicon nitride. Nature 1999, 400: 340–342.
DOI Google Scholar
[2]
Zerr A, Riedel R, Sekine T, et al. Recent advances in new hard high-pressure nitrides. Adv Mater 2006, 18: 2933–2948.
DOI Google Scholar
[3]
Zerr A, Kempf M, Schwarz M, et al. Elastic moduli and hardness of cubic silicon nitride. J Am Ceram Soc 2002, 85: 86–90.
DOI Google Scholar
[4]
Nishiyama N, Ishikawa R, Ohfuji H, et al. Transparent polycrystalline cubic silicon nitride. Sci Rep 2017, 7: 44755.
DOI Google Scholar
[5]
Boyko TD, Hunt A, Zerr A, et al. Electronic structure of spinel-type nitride compounds Si3N4, Ge3N4, and Sn3N4 with tunable band gaps: Application to light emitting diodes. Phys Rev Lett 2013, 111: 097402.
DOI Google Scholar
[6]
Nishiyama N, Langer J, Sakai T, et al. Phase relations in silicon and germanium nitrides up to 98 GPa and 2400 ℃. J Am Ceram Soc 2019, 102: 2195–2202.
DOI Google Scholar
[7]
Jiang JZ, Kragh F, Frost DJ, et al. Hardness and thermal stability of cubic silicon nitride. J Phys-Condens Mat 2001, 13: L515–L520.
DOI Google Scholar
[8]
Tallant DR, Parmeter JE, Siegal MP, et al. The thermal stability of diamond-like carbon. Diam Relat Mater 1995, 4: 191–199.
DOI Google Scholar
[9]
Palmero P. Structural ceramic nanocomposites: A review of properties and powders’ synthesis methods. Nanomaterials 2015, 5: 656–696.
DOI Google Scholar
[10]
Mukhopadhyay A, Basu B. Consolidation–microstructure–property relationships in bulk nanoceramics and ceramic nanocomposites: A review. Int Mater Rev 2007, 52: 257–288.
DOI Google Scholar
[11]
Yue YH, Gao YF, Hu WT, et al. Hierarchically structured diamond composite with exceptional toughness. Nature 2020, 582: 370–374.
DOI Google Scholar
[12]
Bechelany MC, Proust V, Gervais C, et al. In situ controlled growth of titanium nitride in amorphous silicon nitride: A general route toward bulk nitride nanocomposites with very high hardness. Adv Mater 2014, 26: 6548–6553.
DOI Google Scholar
[13]
Kumar A, Gokhale A, Ghosh S, et al. Effect of nano-sized sintering additives on microstructure and mechanical properties of Si3N4 ceramics. Mater Sci Eng A 2019, 750: 132–140.
DOI Google Scholar
[14]
Li W, Li F, Yu ZJ, et al. Polymer-derived SiHfN ceramics: From amorphous bulk ceramics with excellent mechanical properties to high temperature resistant ceramic nanocomposites. J Eur Ceram Soc 2022, 42: 4493–4502.
DOI Google Scholar
[15]
Suffner J, Scherer T, Wang D, et al. Microstructure and high-temperature deformation behavior of Al2O3–TiO2 obtained from ultra-high-pressure densification of metastable powders. Acta Mater 2011, 59: 7592–7601.
DOI Google Scholar
[16]
Solozhenko VL, Kurakevych OO, Le Godec Y. Creation of nanostuctures by extreme conditions: High-pressure synthesis of ultrahard nanocrystalline cubic boron nitride. Adv Mater 2012, 24: 1540–1544.
DOI Google Scholar
[17]
Melaibari AA, Zhao JN, Molian P, et al. Ultrahard boron nitride material through a hybrid laser/waterjet based surface treatment. Acta Mater 2016, 102: 315–322.
DOI Google Scholar
[18]
Colombo P, Mera G, Riedel R, et al. Polymer-derived ceramics: 40 years of research and innovation in advanced ceramics. J Am Ceram Soc 2010, 93: 1805–1837.
DOI Google Scholar
[19]
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.
DOI Google Scholar
[20]
Ionescu E, Terzioglu C, Linck C, et al. Thermodynamic control of phase composition and crystallization of metal-modified silicon oxycarbides. J Am Ceram Soc 2013, 96: 1899–1903.
DOI Google Scholar
[21]
Zhou C, Gao X, Xu Y, et al. Synthesis and high-temperature evolution of single-phase amorphous Si–Hf–N ceramics. J Eur Ceram Soc 2015, 35: 2007–2015.
DOI Google Scholar
[22]
Zhou C. Ternary Si–metal–N ceramics: Single-source-precursor synthesis, nanostructure and properties characterization. Ph.D. Thesis. Darmstadt, Germany: Technical University of Darmstadt, 2017.
[23]
Farla R, Bhat S, Sonntag S, et al. Extreme conditions research using the large-volume press at the P61B endstation, PETRA III. J Synchrotron Radiat 2022, 29: 409–423.
DOI Google Scholar
[24]
Seto Y. PDIndexer 2022. https://github.com/seto77/PDIndexer/.
[25]
Toby BH, Von Dreele RB. GSAS-II: The genesis of a modern open-source all purpose crystallography software package. J Appl Crystallogr 2013, 46: 544–549.
DOI Google Scholar
[26]
Anstis GR, Chantikul P, Lawn BR, et al. A critical evaluation of indentation techniques for measuring fracture toughness: I, Direct crack measurements. J Am Ceram Soc 1981, 64: 533–538.
DOI Google Scholar
[27]
Evans AG, Charles EA. Fracture toughness determinations by indentation. J Am Ceram Soc 1976, 59: 371–372.
DOI Google Scholar
[28]
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.
DOI Google Scholar
[29]
Iwamoto Y, Kikuta KI, Hirano SI. Synthesis of poly-titanosilazanes and conversion into Si3N4–TiN ceramics. J Ceram Soc Jpn 2000, 108: 350–356.
DOI Google Scholar
[30]
Lucovsky G, Yang J, Chao SS, et al. Nitrogen-bonding environments in glow-discharge—Deposited a-Si:H films. Phys Rev B 1983, 28: 3234–3240.
DOI Google Scholar
[31]
Mazzarella L, Kolb S, Kirner S, et al. Optimization of PECVD process for ultra-thin tunnel SiOx film as passivation layer for silicon heterojunction solar cells. In: Proceedings of the 2016 IEEE 43rd Photovoltaic Specialists Conference, Portland, USA, 2016: 2955–2959.
DOI
[32]
Günthner M, Wang KS, Bordia RK, et al. Conversion behaviour and resulting mechanical properties of polysilazane-based coatings. J Eur Ceram Soc 2012, 32: 1883–1892.
DOI Google Scholar
[33]
Tanakaa I, Oba F, Sekine T, et al. Hardness of cubic silicon nitride. J Mater Res 2002, 17: 731–733.
DOI Google Scholar
[34]
Li GX, Rahim MZ, Pan WC, et al. The manufacturing and the application of polycrystalline diamond tools—A comprehensive review. J Manuf Process 2020, 56: 400–416.
DOI Google Scholar
[35]
Monteiro SN, Skury ALD, de Azevedo MG, et al. Cubic boron nitride competing with diamond as a superhard engineering material—An overview. J Mater Res Technol 2013, 2: 68–74.
DOI Google Scholar
[36]
Mattesini M, Ahuja R, Johansson B. Cubic Hf3N4 and Zr3N4: A class of hard materials. Phys Rev B 2003, 68: 184108.
Google Scholar
[37]
Stishov S M, Popova S V. New dense polymorphic modification of silica. Geokhimiya 1962, 8: 649–659.
Google Scholar
[38]
Léger JM, Haines J, Schmidt M, et al. Discovery of hardest known oxide. Nature 1996, 383: 401.
DOI Google Scholar
[39]
Shemkunas MP, Petuskey WT, Chizmeshya AVG, et al. Hardness, elasticity, and fracture toughness of polycrystalline spinel germanium nitride and tin nitride. J Mater Res 2004, 19: 1392–1399.
DOI Google Scholar
[40]
Dzivenko D. High-pressure synthesis, structure and properties of cubic zirconium(IV)- and hafnium(IV) nitrides. Ph.D. Thesis. Darmstadt, Germany: Technical University of Darmstadt, 2009.
[41]
Wang SM, Antonio D, Yu XH, et al. The hardest superconducting metal nitride. Sci Rep 2015, 5: 13733.
DOI Google Scholar
[42]
Chen XJ, Struzhkin VV, Wu ZG, et al. Hard superconducting nitrides. PNAS 2005, 102: 3198–3201.
DOI Google Scholar
[43]
Zhao J, Ai X, Lv ZJ. Preparation and characterization of Si3N4/TiC nanocomposite ceramics. Mater Lett 2006, 60: 2810–2813.
DOI Google Scholar
[44]
Cao MR, Wang SB, Han WB. Influence of nanosized SiC particle on the fracture toughness of ZrB2-based nanocomposite ceramic. Mater Sci Eng A 2010, 527: 2925–2928.
DOI Google Scholar
[45]
Krstic VD. Porosity dependence of strength in brittle solids. Theor Appl Fract Mec 1988, 10: 241–247.
DOI Google Scholar
[46]
Madhav Reddy K, Guo JJ, Shinoda Y, et al. Enhanced mechanical properties of nanocrystalline boron carbide by nanoporosity and interface phases. Nat Commun 2012, 3: 1052.
DOI Google Scholar
[47]
Madhav Reddy K, Guo DZ, Lahkar S, et al. Graphite interface mediated grain-boundary sliding leads to enhanced mechanical properties of nanocrystalline silicon carbide. Materialia 2019, 7: 100394.
DOI Google Scholar
[48]
He DW, Zhao YS, Daemen L, et al. Boron suboxide: As hard as cubic boron nitride. Appl Phys Lett 2002, 81: 643–645.
DOI Google Scholar
[49]
Auerkari P. Mechanical and Physical Properties of Engineering Alumina Ceramics. Espoo, Finland: Valtion teknillinen tutkimuskeskus, 1996.
[50]
Qian J, Daemen LL, Zhao Y. Hardness and fracture toughness of moissanite. Diam Relat Mater 2005, 14: 1669–1672.
DOI Google Scholar
[51]
Filgueira M, Nascimento ÁLN, Oliveira MP, et al. HPHT sintering of binderless Si3N4: Structure, microstructure, mechanical properties and machining behavior. J Braz Soc Mech Sci 2018, 40: 118.
DOI Google Scholar
[52]
Wang CC, Song LL. Nanosheet-structured B4C with high hardness up to 42 GPa. Chin Phys B 2019, 28: 066201.
DOI Google Scholar
[53]
Qin JQ, Nishiyama N, Ohfuji H, et al. Polycrystalline γ-boron: As hard as polycrystalline cubic boron nitride. Scripta Mater 2012, 67: 257–260.
DOI Google Scholar
[54]
Gui R, Xue Z, Zhou XF, et al. Strain stiffening, high load-invariant hardness, and electronic anomalies of boron phosphide under pressure. Phys Rev B 2020, 101: 035302.
DOI Google Scholar
[55]
Drory MD, Ager JW III, Suski T, et al. Hardness and fracture toughness of bulk single crystal gallium nitride. Appl Phys Lett 1996, 69: 4044–4046.
DOI Google Scholar
[56]
Novikov NV, Dub SN. Fracture toughness of diamond single crystals. J Hard Mater 1992, 2: 5–11.
Google Scholar
[57]
Morita K, Kim BN, Hiraga K, et al. Fabrication of high-strength transparent MgAl2O4 spinel polycrystals by optimizing spark-plasma-sintering conditions. J Mater Res 2009, 24: 2863–2872.
DOI Google Scholar
[58]
Ma DJ, Kou ZL, Liu YJ, et al. Sub-micron binderless tungsten carbide sintering behavior under high pressure and high temperature. Int J Refract Met H 2016, 54: 427–432.
DOI Google Scholar
[59]
Dzivenko DA, Zerr A, Miehe G, et al. Synthesis and properties of oxygen-bearing c-Zr3N4 and c-Hf3N4. J Alloys Compd 2009, 480: 46–49.
DOI Google Scholar
[60]
Alexandre N, Desmaison-Brut M, Valin F, et al. Mechanical properties of hot isostatically pressed zirconium nitride materials. J Mater Sci 1993, 28: 2385–2390.
DOI Google Scholar
[61]
Moriyama M, Aoki H, Kobayashi Y, et al. The mechanical properties of hot-pressed TiN ceramics with various additives. J Ceram Soc Jpn 1993, 101: 279–284.
DOI Google Scholar
[62]
Desmaison-Brut M, Montintin J, Valin F, et al. Mechanical properties and oxidation behaviour of HIPed hafnium nitride ceramics. J Eur Ceram Soc 1994, 13: 379–386.
DOI Google Scholar
[63]
Sun RX, Wei XD, Hu WT, et al. Nanocrystalline cubic silicon carbide: A route to superhardness. Small 2022, 18: 2201212.
DOI Google Scholar
[64]
Huang Q, Yu DL, Xu B, et al. Nanotwinned diamond with unprecedented hardness and stability. Nature 2014, 510: 250–253.
DOI Google Scholar
[65]
Liu YJ, He DW, Kou ZL, et al. Hardness and thermal stability enhancement of polycrystalline diamond compact through additive hexagonal boron nitride. Scripta Mater 2018, 149: 1–5.
DOI Google Scholar
[66]
Li W, Du HZ, Tian CM, et al. Single-source-precursor derived bulk Si3N4/HfBxN1−x ceramic nanocomposites with excellent oxidation resistance. Z Anorg Allg Chem 2022, 648: e202200203.
DOI Google Scholar
File
JAC0764_ESM.pdf (1.1 MB)
Publication history
Copyright
Acknowledgements
Rights and permissions

Publication history

Received: 12 February 2023
Revised: 15 April 2023
Accepted: 08 May 2023
Published: 06 July 2023
Issue date: July 2023

Copyright

© The Author(s) 2023.

Acknowledgements

We acknowledge DESY (Hamburg, Germany), a member of the Helmholtz Association of German Research Centres (HGF), for the provision of experimental facilities. Part of this research was carried out at PETRA III LVP at beamline P61B (beamtime I-20200434) and P02.1. Shrikant Bhat and Robert Farla acknowedge the support from the Federal Ministry of Education and Research, Germany (BMBF; Nos. 05K16WC2 and 05K13WC2). Wei Li and Leonore Wiehl also acknowledge the travel support from DESY. Zhaoju Yu thanks the National Natural Science Foundation of China (Nos. 51872246 and 52061135102) for financial support. Marc Widenmeyer and Anke Weidenkaff are grateful for the financial support by the German Ministry of Education and Research (No. 03SF0618B). Wei Li acknowledges the financial support from China Scholarship Council (No. 201907040060).

Rights and permissions

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