- Open Access
Boron nitride nanotubes: synthesis and applications
© The Author(s) 2018
Received: 30 March 2018
Accepted: 15 June 2018
Published: 28 June 2018
Boron nitride nanotube (BNNT) has similar tubular nanostructure as carbon nanotube (CNT) in which boron and nitrogen atoms arranged in a hexagonal network. Owing to the unique atomic structure, BNNT has numerous excellent intrinsic properties such as superior mechanical strength , high thermal conductivity, electrically insulating behavior, piezoelectric property, neutron shielding capability, and oxidation resistance. Since BNNT was first synthesized in 1995, developing efficient BNNT production route has been a significant issue due to low yield and poor quality in comparison with CNT, thus limiting its practical uses. However, many great successes in BNNT synthesis have been achieved in recent years, enabling access to this material and paving the way for the development of promising applications. In this article, we discussed current progress in the production of boron nitride nanotube, focusing on the most common and effective methods that have been well established so far. In addition, we presented various applications of BNNT including polymer composite reinforcement, thermal management packages, piezo actuators, and neutron shielding nanomaterial.
Outstanding and exceptional physical properties of a material can emerge when its size reduces to the nanoscale. Developing nanostructure possessing unique features has always been the essence of nanoscience and nanotechnology since the beginning. Among various nanostructures in general and all kinds of a one-dimensional network in particular, nanotubes have built a strong reputation as the most widely studied nanomaterial. Take carbon nanotube as an example, theoretical and experimental research in every aspect of tubular nanostructure have been flourishing ever since the first discovery of CNT in the early 1990s . CNTs offer numerous fascinating applications in electronic , sensing , composite , and many more are being progressed. The development of new class of nanotube beside the famous carbon allotrope has become an attractive topic in recent years.
Extraordinary and yet distinct characteristics of BNNT have triggered great interest in fundamental studies on properties and applications of this new exotic material. However, unlike research in CNTs which has been well established over a decade, the study on of BNNT is still immature and far less developed than the carbon counterpart. The reason for this situation lies in the synthesis of BNNT which still remains a significant challenge since BNNT was first discovered in 1995 . Whereas the production of high-quality CNT can be easily done in a laboratory with simple equipment, BNNT synthesis require specially designed apparatus in extreme conditions. The lack of efficient synthesis route combining with the high price of readily commercial products could seriously hinder the study of BNNT in the long term. Many remarkable successes in BNNT synthesis have been recently achieved utilizing newly developed and novel techniques. Large quantity and high quality of BNNT are now becoming accessible, and in turn this will gradually foster BNNT research field. In this review, we will present BNNT synthesis methods that are currently widely used, and applications of BNNTs in various area.
2 BNNT synthesis methods
BNNT has been synthesized mainly by methods that have been well documented earlier for CNT fabrication including arc discharge , chemical vapor deposition (CVD) , laser ablation , etc. The essential factor rendering efficient BNNT synthesis process is the rate of conversion from boron and nitrogen sources into BN radicals. Each fabrication technique was scientifically developed in different and distinct strategies, involving specific precursors, conditions, and equipment to promote the growth of BNNT. In this chapter, we will present an overview of various synthesis methods and underline notable features.
2.1 Arc discharge method
2.2 Ball-milling method
Ball milling is a promising technique to synthesize BNNT at industrial scale with low cost. In principle, direct reaction between boron and nitrogen in ambient conditions can be stimulated by introducing defective or amorphous structure in boron starting powders. This transformation is easily done by applying sufficient amount of mechanical energy that is controlled by several parameters such as milling time, and intensity (round per minutes). Therefore, the quantity of BNNT can be immensely produced in a typical run. This process is dependent on the milling time that could be extended to hundreds of hours, and the subsequent annealing of treated boron powder has an essential role in the formation of BNNT.
2.3 Chemical vapor deposition (CVD) method
Chemical vapor deposition (CVD) is one of the most popular ways that have been widely used to produce carbon nanomaterials, and it was lately adopted to synthesize boron nitride materials. In comparison to other approaches, this technique offers better controllability of growth parameters regarding growth mechanism, experimental setup, precursors, catalysts, and temperature, to ensure the high quality of nanomaterials . It is not surprising that CVD process for BNNT growth is relatively similar and reminiscent of CNT synthesis, the differences lie primarily in the types of starting materials, growth conditions. Liquid or solid boron and boron nitride sources are commonly used to grow BNNT instead of toxic and combustible gaseous boron precursors, along with nitrogen gases, such as N2 or NH3. Also, similar to CNT synthesis, transition metal catalysts are particularly efficient at producing BNNT with few layers and small diameter.
Although almost all CVD processes are involved in the use of the catalyst, it is possible that non-catalytic approach can be applied to grow BNNT. Ma et al. attempted to synthesize BNNT using B–N–O precursor generated from melamine diborate (C3N6H6·2H3BO3) . The powder precursor was then rapidly heated and kept in the N2 atmosphere for 2 h. Multi-walled BNNTs formed after the reaction had concentric layers with an inner and outer diameter of 5.2 and 13.1 nm, respectively. The tip of nanotubes was bulbous-like shape encasing B–N–O clusters. In another similar work, BNNT grew directly on α-Al2O3 Å µm-range particles, showing 2–6 concentric layers with slightly larger diameter and partially filled by amorphous B–N–O or boron carbide crystalline .
In contrast to the hundred-gram scale of CNT that can be easily produced, the yield of BNNT obtained in CVD process remains significantly low, typically a couple of 100 mg. Therefore, in pursuance of mass producing BNNT, Tang et al. have developed the so-called boron oxide CVD (BOCVD) in which boron and MgO powder were used as reactants to generate B2O2. BNNTs were subsequently formed via the reaction between B2O2 and NH3 gas at a temperature ranging from 1000 to 1700 °C . The diameter of BNNT formed in this way varied in a wide range from several nanometers to 70 nm, influencing on the constitution of defects. All nanotubes possessed parallel fringe pattern, indicating multi-walled structure with a length up to 10 µm. Gram scale of BNNT having comparable quality can be achieved with the utilization of FeO in the mixture of B and MgO (Fig. 4c–e) . It was later found that Li2O could produce better effects than MgO did on the large-scale production of BNNTs with the reduced diameter of sub-10 nm due to its superior deoxidation capability and pronounced promotion effect on the crystallization of graphite-like BN .
2.4 Laser ablation method
Fabrication of BNNT in laser ablation method has the advantage of producing high-quality nanotubes with a small number of the wall, high aspect ratio, and crystallinity. In this method, a target made of boron or boron nitride undergoes a phase transformation from solid to liquid at a high temperature that exceeds boron melting point (2000 °C) due to laser heating. Thus, direct reaction between surrounding nitrogen atmosphere and boron target can be enhanced efficiently, resulting in the efficient growth of BNNTs. Golberg et al. succeeded in synthesizing BNNT using laser ablation method for the first time . Multi-walled BNNTs were synthesized by laser heating cubic and hexagonal BN targets until 5000 K in a diamond anvil cell in extremely high-pressure (5–15 GPa) of nitrogen gas.
Yu et al. synthesized BNNT by irradiating laser to target prepared by mixing Ni–Co catalyst particles with h-BN powder similar to CNT synthesis . As grown BNNTs had 1–3 layers, and a diameter ranging from 1.5 to 8 nm. Also, through TEM analysis, two types of nanotubes were identified in which BNNT grown with and without catalyst particles nested in tube ends. Zhou et al. confirmed the role of Ni–Co in the following study . In the absence of Ni–Co catalyst, BNNT showed a multi-walled structure with a diameter of 1.5–6 nm and impurities irregularly distributed on the surface of the nanotubes. Whereas in opposite case, most of BNNTs were single walled and impurity free. They explained that the Ni–Co catalyst plays a role in synthesizing high-quality single-walled BNNT.
Lee et al. at Office National d’Etudes et de Recherches Aérospatiales (ONERA) and Centre national de la recherche scientifique (CNRS) in France have developed a method for synthesizing BNNTs using catalyst-free h-BN as a source in by laser ablation . Gram scale of BNNTs (0.6 g/h) was synthesized by heating the target at 3400 K using the continuous CO2 laser in atmospheric nitrogen pressure. The obtained sample consisted of single-walled BNNTs tied into bundles with a length of about 100 nm, besides double and multi-walled tubes. Two ends of nanotube were either encapsulated by boron nanoparticles or flat-closed. This evidence suggests that the formation of BNNT can follow root growth mechanism. Besides, the growth of single-walled BNNTs without catalyst was also confirmed. Next, in another study conducted by Arenal et al. in ONERA-CNRS, BNNTs were produced by continuously heating pressed a mixture of h-BN powder and boron oxide binder as a target in nitrogen partial pressure conditions . The amount of single-walled BNNTs, in this case, was account for roughly 80% in final products, and tube length was several 100 nm. From the analysis of boron nanoparticle enclosed by h-BN layer, it was found that oxygen impurities could restrain the formation of BNNT. In situ diagnostic methods developed by Cau et al. using the UV-laser induced fluorescence (LIF) and UV–Rayleigh scattering (RS) indicate the existence of BN and BO species in the plume above heated h-BN target . The results supported the root growth mechanism and confirm the inhibition of BNNT growth due to oxygen impurities in previous studies. Therefore, to increase the yield of BNNT, pure boron and nitrogen sources are highly required.
2.5 Thermal plasma jet method
Though BNNTs produced by laser ablation technique possessed very high structural quality, the production rate is still limited, under a milligram per hour, due to the confinement of growth area in a small volume. Thermal plasma methods seem to be an alternative solution to this issue, since it is capable of applying high thermal energy over a wider volume, extending growth area of BNNTs up to hundreds square centimeters. Plasma jet, one of the thermal plasma-based methods, consists of two concentric electrodes anode and cathode. The plasma generated when a gas mixture (Ar, N2, H2) flows in between two electrodes pass through a nozzle, forming a broad region of arc plasma jet .
Shimizu et al. prepared multi-walled BNNTs by heating a sintered BN target in a plasma jet (DC power of 8 kW, Ar–H2 mixed gas) at 100 Torr (~ 4000 K) . The results indicated a strong correlation of high-temperature conditions with mass production of BNNT in this method. Through the TEM analysis, some initial evidence on the growth direction and mechanism of BNNT from phase boundaries existing at the opposite ends of nanotube was given. Lee et al. synthesized BNNTs by continuously injecting a powder mixture of h-BN and Ni/Y catalyst particles into a plasma jet (DC power of 14 kW, Ar–N2 mixed gas) at atmospheric pressure (5000–20000 K) . Though most of the BNNTs were identified as multi-walled with diameters ranging from 3 to 10 nm, single and double walled BNNTs were also observed.
2.6 BNNT applications
Based on various unique properties, BNNTs have great potential for practical uses in many areas. Despite limitations on fabrication technique, there is an increasing number of fundamental studies, suggesting and developing BNNT applications. Significant successes have been achieved, and in most case, BNNT is conclusively proved to be a promising candidate for mechanical reinforcement in the nanocomposite and advanced functional materials.
At present, the research study on practical uses of BNNT is extensively and continually conducted. For instance, in water purification, BNNTs has been examined in oil-filtering , self-cleaning membranes , and reusable heat-resistive films . In the field of biological application, due to the nontoxicity property, BNNTs can be used as a biological probe , drug carrier , or biological channel in biosensor . High stability towards oxidation of BNNTs has enabled its access to field emission technology [75, 76]. In addition, BNNT has also been reported in hydrogen storage [77–80], sensing [81, 82], and optoelectronic [83, 84]. It is highly anticipated that the application of BNNT will continue to extend in the future.
Major achievements in the production of boron nitride nanotube in recent times are the favorable outcome of the development of novel approaches including boron oxide-chemical vapor deposition (BOCVD), thermal plasma, and high temperature–pressure laser ablation. The typical strategy sharing among these methods is to stimulate the direct reaction between boron and nitrogen precursors. This can be done systematically by several ways such as creating highly disorder or amorphous structure in starting materials (ball milling), utilizing effective catalysts (floating catalyst CVD), and producing gas-phase (BOCVD) or liquid-phase (HPC laser ablation) reaction between boron and nitrogen gas. Although the quality and quantity of BNNT have been significantly improved, these approaches also exert side effects, for example, undesirable formation of amorphous boron, boron nitride, and h-BN, thus, leading to the degradation of BNNT purity. To tackle this problem, besides developing an efficient purification process, optimizing synthesis method is critically important. However, in doing so, it requires a profound understanding of the growth mechanism of BNNT in every single method. Recently, computer simulation and in situ diagnostic tools to evaluate every critical factor from several research groups have initially provided some insight into growing process of BNNT [51, 53, 58]. On the other hand, the widespread availability of BNNT has triggered great interest in the development of BNNT applications. The effectiveness of BNNT has been promisingly approved in reinforcing polymeric composite, boosting thermal managing capability of electronic devices, and enhancing neutron shielding in aerospace. Although the BNNT-related technology is still in its infancy, it is expected that many more fascinating applications will be developed in years to come.
JHK wrote the manuscript and MJK guided manuscript preparation. TVP and JHH helped writing the manuscript. CSK gave corrections to enhance the manuscript quality. All authors read and approved the final manuscript.
This work was supported by a Grant from the KIST 4U ORP (Open Research Program).
The authors declare that they have no competing interests.
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