Synthesis and structure–property relationships of a new family of layered carbides in Zr-Al(Si)-C and Hf-Al(Si)-C systems

doi:10.1016/j.jeurceramsoc.2013.05.020

Journal of the European Ceramic Society

Volume 33, Issues 15–16, December 2013, Pages 2831-2865

https://doi.org/10.1016/j.jeurceramsoc.2013.05.020 Get rights and content

Abstract

The layered ternary and quaternary carbides in Zr-Al(Si)-C and Hf-Al(Si)-C systems with general formulae of (TC)_nAl₃C₂, (TC)_nAl₄C₃ and (TC)_n[Al(Si)]₄C₃ (where T = Zr or Hf, n = 1, 2, 3…) have attracted increasing attentions due to their fascinating properties such as high specific stiffness, high strength and fracture toughness, refractory, machinability by electrical discharge method, thermal shock resistance, as well as high-temperature and ultrahigh-temperature oxidation resistance. The combination of these properties makes them promising as structural components or coatings for high- and ultrahigh-temperature applications. In this review, the progresses on processing, and structure–property relationships of the novel layered carbides are comprehensively outlined. The crystal structure characteristics are introduced first. Then, methods for processing powders and bulk samples are summarized. The third section focuses on the multi-scale structure–property relationships. Finally, the potential applications and further trends in tailoring the properties and developing low cost processing methods are highlighted.

Introduction

Transition metal carbides (TMCs), such as ZrC, HfC, TaC, and TiC display high melting point, high hardness, good wear resistance and chemical inertness, excellent thermal and electrical conductivities, and absence of phase transformations in solid states. These merits make TMCs promising in applications in extreme environments such as in re-entry vehicle, rocket/scramjet engine, thermal protecting system for hypersonic vehicles, and structural and fuel matrix materials in generation IV nuclear reactors.1, 2, 3, 4 However, intrinsic brittleness and poor oxidation resistance are the two main concerns that provide TMCs low reliability. Inspired by the recent progresses of the well-known TAX phases (also referred as the MAX phase in literature, here we use T instead of M for consistency with other transition metal carbides; the general formula of TAX phase is T_n+1AX_n, where T is an early transition metal, A is an A group element, X is either C and/or N, n = 1, 2, 3…), incorporating Al into the binary carbides might significantly improve the ductility and oxidation resistance.5, 6, 7 For instances, Ti₃AlC₂, Ti₂AlC, and Cr₂AlC are good examples of TAX phases,8, 9 which exhibit excellent oxidation resistance and damage tolerance besides other merits such as high strength and modulus, high thermal and electrical conductivities, excellent thermal shock resistance, high reliability and machinability shared by other TAX phases. For details of the crystal structure and properties of TAX phases, please refer to recent reviews published by various research groups.5, 6, 7, 8, 9, 10, 11 Unfortunately, TAX phases have not yet been discovered in either Zr-Al-C or Hf-Al-C system.⁵ Recently, a new family of layered ternary and quaternary compounds with the general formula of (TC)_nAl₃C₂ and (TC)_n[Al(Si)]₄C₃ (where T = Zr or Hf, n = 1, 2, 3…) was developed in Zr-Al(Si)-C and Hf-Al(Si)-C systems: some of the ternary carbides were discovered early in 1980s by Michalenko et al.,¹² and Schuster and Nowotny,¹³ and their crystal structures were reported by Parthé and Chabot,¹⁴ as well as by Gesing and Jeitschko.¹⁵ Compared to TAX phases, the crystal structures of (TC)_nAl₃C₂ and (TC)_n[Al(Si)]₄C₃ compounds can be described as ZrC_x or HfC_x blocks being interleaved by Al₃C₂ or [Al(Si)]₄C₃ unit. These (TC)_nAl₃C₂ and (TC)_n[Al(Si)]₄C₃ materials also showed interesting physical and mechanical properties as well as the high temperature oxidation resistance. In the past six years, besides the vigorous progress towards developing new synthesis methods and understanding physical and mechanical properties, a number of new compounds belonging to this family have been discovered. In this review, recent progresses on novel processing, multi-scale structure features and properties of ternary carbides (TC)_nAl₃C₂ and quaternary (TC)_n[Al(Si)]₄C₃ (T = Zr, Hf, n = 1,2,3,4,…) are summarized. The first section focuses on the crystal structures of these layered carbides. The second section summarizes synthesis methods of powders and bulk materials of layered Zr-Al(Si)-C and Hf-Al(Si)-C carbides. In the third section, their electronic structure and microstructure features will be described. In the fourth section, the physical and mechanical properties as well as the high temperature oxidation behavior of (TC)_nAl₃C₂ and (TC)_n[Al(Si)]₄C₃ carbides will be reviewed. Finally, an outlook of the potential applications of (TC)_nAl₃C₂ and (TC)_n[Al(Si)]₄C₃ and future trends in improving the properties of these fascinating materials will be highlighted.

Section snippets

Crystal structures of ternary (TC)_nAl₃C₂ and quaternary (TC)_n[Al(Si)]₄C₃ carbides

Before describing the crystal structures of ternary carbides (TC)_nAl₃C₂ and quaternary carbides (TC)_n[Al(Si)]₄C₃ in Zr-Al(Si)-C and Hf-Al(Si)-C systems, it is helpful to introduce the crystal structure of T _n+1AX_n (n = 1,2,3,4,5,…) phases. The crystal structures of TAX phases crystallize in the hexagonal symmetry and consist of two basic units, i.e., the non-stoichiometric T_n+1X_n units and atomic planes of A atoms. The difference between crystal structures of T_n+1AX_n compounds is the thickness of

Preparation of layered ternary carbides in Zr-Al-C system

Synthesis of layered ternary Zr-Al-C ceramics is an essential step to investigate the structure and properties of these materials. However, works on the preparation of Zr-Al-C powders and bulk ceramics were not extensively conducted until very recently. Methods used for the synthesis and densification of Zr-Al-C ceramics include arc-melting,¹³ solid state reaction,30, 31 pulse electric current sintering (PECS),³² solid–liquid reaction,³³ and reactive hot pressing.34, 35 The main methods used

Electronic structure, chemical bonding and intrinsic properties of Zr-Al(Si)-C and Hf-Al(Si)-C carbides

The crystal structure features of layered carbides in Zr-Al(Si)-C and Hf-Al(Si)-C systems have been summarized in section II, so in this section we will emphasize the electronic structure and microstructure of these new materials. Since the electronic structure and chemical bonding nature underpin the properties of materials, it is of vital importance to investigate the electronic structure of layered carbides in Zr-Al(Si)-C and Hf-Al(Si)-C systems first. The electronic band structure, chemical

Mechanical, thermal and oxidation resistance of Zr-Al(Si)-C and Hf-Al(Si)-C carbides

Due to the difficulty in synthesizing single phase and dense bulk materials, the properties of Zr-Al(Si)-C and Hf-Al(Si)-C ceramics were not extensively investigated until very recently. Leela-Adisorn et al.30, 49 first reported the preliminary properties of Zr₂Al₃C₄ and Zr₃Al₃C₅ ceramics, then He et al.35, 36, 39, 46 systematically investigated the mechanical, thermal and oxidation properties of Zr₂Al₃C₄, Zr₃Al₃C₅, Zr₂[Al(Si)]₄C₅, Zr₃[Al(Si)]₄C₆, Hf₂[Al(Si)]₄C₅ and a Hf-Al-C composite. The

Potential applications and further trends in developing Zr-Al(Si)-C and Hf-Al(Si)-C carbides

Zr-Al(Si)-C and Hf-Al(Si)-C carbides are refractory, light weight, thermal and electrical conductive, machinable by the electrical discharge method, and resistant to high temperature and ultrahigh temperature oxidation and thermal shock. They also have better mechanical properties than their binary counterparts ZrC and HfC, e.g., high specific stiffness, stable stiffness up to 1650 °C, and high fracture toughness and strength. The unique combination of these merits ensures Zr-Al(Si)-C and

Conclusion remarks

In this review, the crystal structure, electronic structure, microstructure characters and physical, mechanical properties as well as oxidation behavior of recently developed layered ternary carbides (TC)_nAl₃C₂, (TC)_n(Al₄C₃)_n and quaternary carbides (TC)_n[Al(Si)]₄C₃ (T = Zr or Hf, n = 2, 3…) are summarized. The crystal structure of these carbides can be described as transition metal carbide TC layers interleaved by Al₃C₂, Al₄C₃ or [Al(Si)]₄C₃ structure unit. Because of the small lattice mismatch,

Acknowledgments

This work was supported by the National Outstanding Young Scientist Foundation for Y C Zhou under Grant No. 59925208, and the Natural Sciences Foundation of China under Grant Nos. 50672102, 50832008, 51032006 and 91226202.

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Yan-Chun Zhou is a professor and deputy director of Science and Technology on Advanced Functional Composites, Aerospace Research Institute of Material & Processing Technology. He obtained his BS from Tsinghua University, MS and PhD degree from Institute of Metal Research, Chinese Academy of Sciences. Before joining ARIMP, he was Professor and Director of High-performance Ceramic Division, Shenyang National Laboratory for Materials Science until 2010. His main research interests are designing, processing and understanding the structural-property relations of damage tolerant ceramics for high and ultrahigh temperature applications. He has published over 320 peer-reviewed papers and holds 30 Chinese patents. He received the Global Star Award from the American Ceramic Society in 2010 and was elected Academician of the World Academy of Ceramics in 2009 and Fellow of the American Ceramic Society in 2010.

Ling-Feng He is now a postdoctoral research associate at University of Wisconsin-Madison, Wisconsin, USA. Dr He received a BEng degree in Metallurgical Science and Engineering at Central South University in China in 2003 and a PhD degree in materials science at University of Chinese Academy of Sciences in China in 2009. His PhD work focused on the synthesis, microstructure and properties of ternary carbides in Zr-Al-C and Hf-Al-C systems. He then worked as a postdoctoral research associate at the Extreme Energy-Density Research Institute at Nagaoka University of Technology, Japan, where he focused on synthesis and characterization of structural and functional ceramic nanocomposites. In 2011, He joined the nuclear fuel and material research group in University of Wisconsin-Madison, where he has been studying the irradiation behavior of nuclear fuels and corrosion behavior of steels and Ni-based alloys using advanced microscopy techniques. He has authored/co-authored over 40 technical papers and holds 4 patents.

Zhi-Jun Lin has over 10 years’ experience in materials science and is the author of more than 60 scientific papers. Following a PhD in materials science (with focus on layered ternary ceramics) at Institute of Metal Research, Chinese Academy of Sciences, he took a postdoctoral research associate position in Los Alamos National Laboratory, where he performed some experimental/theoretical work on hard/superhard materials. Dr Lin also had been a research scientist in Carnegie Institution of Washington for a few months. Currently, he's a Polycrystalline Diamond Compact (PDC) cutter R&D engineer in Schlumberger.

Jing-Yang Wang is a professor of ceramic science and engineering and deputy director of the High-performance Ceramics Division at the Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences. His main research interests include integrated theoretical and experimental investigations of nano-laminated carbides and nitrides for extreme environmental applications and advanced materials for thermal insulation applications. He has authored/co-authored over 130 scientific papers (with the H-index of 27) and holds 10+ patents in the field of ceramics. Prof. Wang was honored with the Global Star Award by the American Ceramic Society in 2012 and the National Science and Technology Progress Award in 2011.

¹: Present address: Department of Engineering Physics, University of Wisconsin-Madison, WI53705, USA.

²: Present address: PDC Cutters R&D, Smith Bits, Schlumberger 1310 Rankin Road, Houston, TX 77073, USA.

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Feature articleSynthesis and structure–property relationships of a new family of layered carbides in Zr-Al(Si)-C and Hf-Al(Si)-C systems

Abstract

Introduction

Section snippets

Crystal structures of ternary (TC)nAl3C2 and quaternary (TC)n[Al(Si)]4C3 carbides

Preparation of layered ternary carbides in Zr-Al-C system

Electronic structure, chemical bonding and intrinsic properties of Zr-Al(Si)-C and Hf-Al(Si)-C carbides

Mechanical, thermal and oxidation resistance of Zr-Al(Si)-C and Hf-Al(Si)-C carbides

Potential applications and further trends in developing Zr-Al(Si)-C and Hf-Al(Si)-C carbides

Conclusion remarks

Acknowledgments

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Sintering and mechanical properties of AlZrC2

J Ceram SoC Jpn

Synthesis and oxidation of Zr3Al3C5 powders

Feature article
Synthesis and structure–property relationships of a new family of layered carbides in Zr-Al(Si)-C and Hf-Al(Si)-C systems

Crystal structures of ternary (TC)_nAl₃C₂ and quaternary (TC)_n[Al(Si)]₄C₃ carbides

Current status in layered ternary carbide Ti₃SiC₂, a review

Synthesis, microstructure, and properties of Cr₂AlC

New ternary carbides ZrAlC_2−x and HfAlC_2−x and their crystal structure

Zr₂Al₃C_5−x and Hf₂Al₃C_5−x described with higher symmetrical space group P6₃/mmc

Ab initio calculation of titanium silicon carbide (Ti₃SiC₂)

Ab-initio geometry optimization and ground state properties of layered ternary carbides Ti₃MC₂(M = Al, Si, Ge)

Synthesis, crystal structure, and thermoelectric properties of a new carbide Zr₃[Al_3.56Si_0.44]C₆

Synthesis and crystal structure of a new layered carbide ZrAl₄C₄

Synthesis and crystal structure of a new layered carbide ZrAl₈C₇

Crystal structure and theoretical elastic property of a new ternary ceramic HfAl₄C₄

Synthesis of Zr₂Al₃C₅ material

AlZrC₂ synthesis

Sintering and mechanical properties of AlZrC₂

Synthesis and oxidation of Zr₃Al₃C₅ powders

Crystal structure of Zr₂Al₃C₄

Synthesis, physical and mechanical properties of bulk Zr₃Al₃C₅ ceramic