Elsevier

Ceramics International

Volume 48, Issue 6, 15 March 2022, Pages 7344-7361
Ceramics International

Zirconium-diboride silicon-carbide composites: A review

https://doi.org/10.1016/j.ceramint.2021.11.314Get rights and content

Abstract

Zirconium diboride (ZrB2) and silicon carbide (SiC) composites have long been of interest since it was observed that ZrB2 improved the thermal shock resistance of SiC. However, processing of these materials can be difficult due to high and different sintering temperatures and differences in the thermodynamic stability of each material. ZrB2–SiC composites have been processed in a variety of ways including hot-pressing, spark-plasma sintering, reactive melt infiltration, pack cementation, chemical vapor deposition, chemical vapor infiltration, stereolithography, direct ink writing, selective laser sintering, electron beam melting, and binder jet additive manufacturing. Each manufacturing method has its own pros and cons. This review serves to summarize more than 60 years of research and provide a coherent resource for the variety of methods and advancements in development of ZrB2–SiC composites.

Introduction

It was documented as early as 1956, that addition of about 30 weight percent (wt%) zirconium diboride (ZrB2) improved the thermal shock resistance of silicon carbide (SiC) [1]. In 1966, it was documented that additions of SiC (up to 20 volume percent (vol%)) improved the oxidation rate of ZrB2 significantly [2]. It has latter been shown that 20–30 vol% SiC in ZrB2 provides optimal oxidation resistance, where this range is dependent on particle size [3] and interconnectivity of the secondary phase network [4]. Since these findings, there has been significant interest in this composite material for harsh-environment applications. Individually, these materials are advantageous due to their room- and high-temperature mechanical and chemical performance. ZrB2 has high melting temperature (3245 °C) [2], high hardness (23 GPa) [2], high strength (337–398 MPa) [5], moderate fracture toughness (3.5 MPa m1/2) [6], and retains mechanical performance at elevated temperatures (1600 °C) in air [7]. SiC also has high melting temperature (2830 °C) [8], high hardness (19.8 GPa) [9] and strength (224 GPa) [9], but has low fracture toughness (2.3 MPa m1/2) [10]. Composites of these two have been shown to have improved strength [[11], [12], [13]], fracture toughness [11,12,14], and hardness [11,13,15]. Additionally, ZrB2 benefits from SiC addition through the formation of a borosilicate glass layer during oxidation, which slows oxygen diffusion to unaffected ZrB2–SiC layers thus protecting the material below the oxide layer [[16], [17], [18], [19], [20]], under certain environmental conditions [17]. These properties have made these composites advantageous for use in refractory and aerospace applications [2,[21], [22], [23]]. However, fabricating these materials into useful shapes is difficult for the same reasons they are desired: mechanical and chemical stability at high temperatures.

ZrB2–SiC composites have been processed in a variety of ways including hot-pressing, pressureless sintering, spark-plasma sintering, flash sintering, combustion synthesis, reactive melt infiltration, pack cementation, chemical vapor deposition, chemical vapor infiltration, stereolithography, direct ink writing, selective laser sintering, electron beam melting, and binder jet additive manufacturing. Each process has its own unique benefits/drawbacks and thus, different considerations for fabricating components for a specific application. The goal of this paper is to summarize ZrB2–SiC processing techniques and identify new research directions.

Section snippets

Bulk solid fabrication techniques

Historically [24], densification of ZrB2 (and hafnium diboride, HfB2) was only attainable by hot pressing at extremely high temperatures and moderate pressures (>2100 °C, 30–40 MPa) [[25], [26], [27]] or high temperatures and extreme pressures (1800 °C, 827–1500 MPa) [28,29]. Since the late 1980's, additional development of ultra-high temperature materials has resulted in reduced temperatures and pressures being required to attain high densification by using sintering aids. However, even with

Deposition and infiltration techniques

Zirconium diboride and zirconium diboride-silicon carbide composite and coating structures have been in development since the early stages of efforts to create vehicles for space travel and have been processed using virtually all known deposition and infiltration techniques. ZrB2–SiC coatings have been deposited on C–C composites, to provide oxidation protection using techniques such as thermal spray, pack cementation, slurry deposition, liquid precursor infiltration, melt infiltration and

Additive manufacturing methods

Only one study on additive manufacturing on ZrB2–SiC composites has been published. In addition to the limited information on AM of ZrB2–SiC, the review will present relevant research results for AM of SiC and for ZrB2 individually. Because there are a variety of AM studies documenting AM of SiC, Table 1 is provided to summarize recent advances, identify remaining gaps, and provide insight for potential relevance to fabricating ZrB2–SiC composites.

The AM of ZrB2–SiC composites has focused on

Sintering aids

The goal of any sintering process is to reduce porosity and increase density, typically to as near to 100% as possible. Because ceramic materials require very high temperatures to densify, processes are often employed to lower the energy (sintering time, temperature, and pressure) required to achieve high density. Materials with a high level of covalent bonding, such as SiC–ZrB2 [190]composites, are even more challenging to sinter, due to their low interdiffusion rates. Sintering is heavily

Summary

Research on the bulk fabrication of dense ZrB2 and ZrB2-based ceramics has investigated a variety of sintering techniques. While once considered unsinterable, fully densified and fine-grained materials with ZrB2 are now attainable at temperatures below 2000 °C with and without external pressure. From the survey of several bulk fabrication techniques for ZrB2 and ZrB2-based composite ceramics, there are several successful strategies applicable to improve densification. These include using

Suggestions for future development

Densification of ZrB2–SiC materials could benefit from a more thorough characterization of the effect of particle size on final density and mechanical properties, with consideration of the end-use environment. As grain size is an important parameter for both powder sinterability and ultimate mechanical properties, determining both initial (after ball-milling but before sintering) and final, sintered particle sizes is critical for complete material characterization and repeatability for other

Funding

This work was supported by the DOE Office of Energy Efficiency and Renewable Energy, Advanced Manufacturing Offices. Research sponsored by the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory, managed by UT-Battelle, LLC for the US Department of Energy under contract DE-AC05-00OR22725 (LOIS Project ID: 10572, Additive manufacturing of ceramics for harsh environments).

Declaration of competing interest

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

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    This manuscript has been authored by UT-Battelle LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan).

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