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1.
RSC Adv ; 12(25): 16291-16295, 2022 May 23.
Artigo em Inglês | MEDLINE | ID: mdl-35733664

RESUMO

Approximately 30% of as-grown carbon nanotube (CNT) networks are metallic, usually leading to a trade-off between carrier mobility and on/off ratio in CNT thin-film transistors (TFTs). Figuring out the key factors of ultra-high on/off ratio in CNT TFTs should be considerably essential for the development of large-scale electronic devices in the future. Here ultra-high on/off ratios of 107-108 are realized for CNT TFTs with mobility of ∼500 cm2 V-1 s-1. We propose that one of the key factors to achieve the high on/off ratio is a clean CNT thin film without charge traps and doping due to residual dispersant used in conventional solution processes. Moreover, on/off ratio degradation under operation voltage is significantly suppressed by decreasing the diameter of CNTs.

2.
Proc Natl Acad Sci U S A ; 118(37)2021 Sep 14.
Artigo em Inglês | MEDLINE | ID: mdl-34508003

RESUMO

We recently synthesized one-dimensional (1D) van der Waals heterostructures in which different atomic layers (e.g., boron nitride or molybdenum disulfide) seamlessly wrap around a single-walled carbon nanotube (SWCNT) and form a coaxial, crystalized heteronanotube. The growth process of 1D heterostructure is unconventional-different crystals need to nucleate on a highly curved surface and extend nanotubes shell by shell-so understanding the formation mechanism is of fundamental research interest. In this work, we perform a follow-up and comprehensive study on the structural details and formation mechanism of chemical vapor deposition (CVD)-synthesized 1D heterostructures. Edge structures, nucleation sites, and crystal epitaxial relationships are clearly revealed using transmission electron microscopy (TEM). This is achieved by the direct synthesis of heteronanotubes on a CVD-compatible Si/SiO2 TEM grid, which enabled a transfer-free and nondestructive access to many intrinsic structural details. In particular, we have distinguished different-shaped boron nitride nanotube (BNNT) edges, which are confirmed by electron diffraction at the same location to be strictly associated with its own chiral angle and polarity. We also demonstrate the importance of surface cleanness and isolation for the formation of perfect 1D heterostructures. Furthermore, we elucidate the handedness correlation between the SWCNT template and BNNT crystals. This work not only provides an in-depth understanding of this 1D heterostructure material group but also, in a more general perspective, serves as an interesting investigation on crystal growth on highly curved (radius of a couple of nanometers) atomic substrates.

3.
Adv Sci (Weinh) ; 8(7): 2004092, 2021 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-33854897

RESUMO

Recently, foldable electronics technology has become the focus of both academic and industrial research. The foldable device technology is distinct from flexible technology, as foldable devices have to withstand severe mechanical stresses such as those caused by an extremely small bending radius of 0.5 mm. To realize foldable devices, transparent conductors must exhibit outstanding mechanical resilience, for which they must be micrometer-thin, and the conducting material must be embedded into a substrate. Here, single-walled carbon nanotubes (CNTs)-polyimide (PI) composite film with a thickness of 7 µm is synthesized and used as a foldable transparent conductor in perovskite solar cells (PSCs). During the high-temperature curing of the CNTs-embedded PI conductor, the CNTs are stably and strongly p-doped using MoO x , resulting in enhanced conductivity and hole transportability. The ultrathin foldable transparent conductor exhibits a sheet resistance of 82 Ω sq.-1 and transmittance of 80% at 700 nm, with a maximum-power-point-tracking-output of 15.2% when made into a foldable solar cell. The foldable solar cells can withstand more than 10 000 folding cycles with a folding radius of 0.5 mm. Such mechanically resilient PSCs are unprecedented; further, they exhibit the best performance among the carbon-nanotube-transparent-electrode-based flexible solar cells.

4.
ACS Nano ; 15(5): 8418-8426, 2021 May 25.
Artigo em Inglês | MEDLINE | ID: mdl-33881302

RESUMO

Single-walled and multiwalled molybdenum disulfide (MoS2) nanotubes have been coaxially synthesized on small-diameter boron nitride nanotubes (BNNTs) that are obtained from removing single-walled carbon nanotubes (SWCNTs) in heteronanotubes of SWCNTs coated by BNNTs. The photoluminescence (PL) from single-walled MoS2 nanotubes supported by core BNNTs is observed in this work, which evidences the direct bandgap structure of single-walled MoS2 nanotubes with a diameter around 6-7 nm. The observation is consistent with our DFT results that the single-walled MoS2 nanotube changes from an indirect-gap to a direct-gap semiconductor when the diameter of a nanotube is more than around 5.2 nm. On the other hand, when there are SWCNTs inside the heteronanotubes of BNNTs and single-walled MoS2 nanotubes, the PL signal from MoS2 nanotubes is considerably quenched. The charge transfer and energy transfer between SWCNTs and single-walled MoS2 nanotubes were examined through characterizations by PL, X-ray photoelectron spectroscopy, and Raman spectroscopy. Moreover, the PL signal from multiwalled MoS2 nanotubes is significantly quenched. Single-walled and multiwalled MoS2 nanotubes exhibit different Raman features in both resonant and nonresonant Raman spectra.

5.
Nanotechnology ; 32(20): 205708, 2021 May 14.
Artigo em Inglês | MEDLINE | ID: mdl-33513593

RESUMO

The thermal properties of individual single-walled carbon nanotubes (SWCNTs) have been well documented in the literature following decades of intensive study. However, when SWCNTs form a macroscale assembly, the thermal transport in these complex structures usually not only depends on the properties of the individual tubes, but also is affected and sometimes dominated by inner structural details, e.g. bundles and junctions. In this work, we first performed an experimental measurement of the thermal conductivities of individual SWCNT bundles of different sizes using a suspended micro-thermometer. The results, together with the data that we obtained from a previous work, give a complete experimental understanding of the effect of bundling on the thermal conductivity of SWCNTs. With these quantitative understandings, we propose a phenomenological model to describe the thermal transport in two-dimensional (2D) SWCNT films. The term 'line density' is defined to describe the effective thermal transport channels in this complex 2D network. Along with experimentally obtained geometric statistics and film transparency, the thermal conductance of SWCNTs is estimated, and the effects of bundle length, diameter, and contact conductance are systematically discussed. Finally, we extend this model to explain thermal transport in 2D networks of one-dimensional van der Waals heterostructures, which are coaxial hetero-nanotubes we recently synthesized using SWCNTs as the template. This extended model suggests that the contribution of boron nitride nanotubes (BNNTs) to the overall performance of a SWCNT-BNNT heterostructured film depends on the transparency of the original SWCNT film. The increase in the thermal conductance of a highly transparent film is estimated to be larger than that of a less transparent film, which shows a good agreement with our experimental observations and proves the validity of the proposed phenomenological model.

6.
Adv Mater ; 33(8): e2006395, 2021 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-33314478

RESUMO

Although single-wall carbon nanotubes (SWCNTs) exhibit various colors in suspension, directly synthesized SWCNT films usually appear black. Recently, a unique one-step method for directly fabricating green and brown films has been developed. Such remarkable progress, however, has brought up several new questions. The coloration mechanism, potentially achievable colors, and color controllability of SWCNTs are unknown. Here, a quantitative model is reported that can predict the specific colors of SWCNT films and unambiguously identify the coloration mechanism. Using this model, colors of 466 different SWCNT species are calculated, which reveals a broad spectrum of potentially achievable colors of SWCNTs. The calculated colors are in excellent agreement with existing experimental data. Furthermore, the theory predicts the existence of many brilliantly colored SWCNT films, which are experimentally expected. This study shows that SWCNTs as a form of pure carbon, can display a full spectrum of vivid colors, which is expected to complement the general understanding of carbon materials.

7.
Nanoscale ; 12(42): 21923-21931, 2020 Nov 05.
Artigo em Inglês | MEDLINE | ID: mdl-33112348

RESUMO

The structure and phase transformation of a cobalt (Co) catalyst, during single walled carbon nanotube (SWCNT) growth, is elucidated for inactive, active and deactivated nanoparticles by in situ imaging using an environmental transmission electron microscope. During nanotube growth, the structure was analyzed using Miller indices to determine the types of planes that favor anchoring or liftoff of nanotubes from the Co catalyst. Density functional theory was further applied to model the catalyst interactions to compare the work of adhesion of the catalyst's faceted planes to understand the interactions of different Miller planes with the graphene structure. Through in-depth studies of multiple distinct Co nanoparticles, we established a dominant nanoparticle phase for SWCNT growth. In addition, we identified the preferred lattice planes and a threshold for work of adhesion to allow the anchoring and liftoff of SWCNTs.

8.
Adv Mater ; 32(39): e2004277, 2020 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-32851708

RESUMO

Single-walled carbon nanotube (SWCNT) films are promising materials as flexible transparent conductive films (TCFs). Here, inspired by the extrusion blown plastic film technique and the SWCNT synthesis approach by floating catalyst chemical vapor deposition (FCCVD), a novel blown aerosol chemical vapor deposition (BACVD) method is reported to directly and continuously produce freestanding SWCNT TCFs at several hundred meters per hour. The synthesis mechanism, involving blowing a stable aerosol bubble and transforming the bubble into an aerogel, is investigated, and a general phase diagram is established for this method. For the SWCNT TCFs via BACVD, both carbon conversion efficiency and SWCNT TCF yield can reach three orders of magnitude higher than those with the conventional FCCVD. The film displays a sheet resistance of 40 ohm sq-1 at 90% transmittance after being doped, representing the record performance based on large-scale SWCNT films. Transparent, flexible, and stretchable electrodes based on BACVD films are demonstrated. Moreover, this high-throughput method of producing SWCNT TCFs can be compatible with the roll-to-roll process for mass production of flexible displays, touch screens, solar cells, and solid-state lighting, and is expected to have a broad and long-term impact on many fields from consumer electronics to energy conversion and generation.

9.
Nanoscale ; 12(23): 12263-12267, 2020 Jun 18.
Artigo em Inglês | MEDLINE | ID: mdl-32495811

RESUMO

Here, a scalable floating catalyst chemical vapor deposition (FCCVD) method is developed for the production of single-walled carbon nanotubes (SWCNTs) with a controlled structure. For the first time, water is used as the growth promoter in the FCCVD process to modulate the growth of SWCNTs. At an optimum water concentration of ca. 115 ppm, the water-assisted FCCVD process synthesizes SWCNTs with a significantly narrow chirality distribution. In particular, the proportion of (9,8) and (8,7) semiconducting tubes was dramatically enhanced to 45% with 27% of the (9,8) tube in the end product. This is attributed to the changes in both the SWCNT diameter and the chiral angle. The experiment results and accurate quantum chemical molecular dynamics simulations show that the addition of water affects the nucleation and the size distribution of nanoparticle catalysts, thus resulting in the growth of SWCNTs with a highly uniform structure. This direct and continuous water-assisted FCCVD provides the possibility for the mass production of high-quality SWCNTs with a controlled structure.

10.
Anal Chem ; 92(12): 8218-8227, 2020 06 16.
Artigo em Inglês | MEDLINE | ID: mdl-32412733

RESUMO

Oxycodone is a strong opioid frequently used as an analgesic. Although proven efficacious in the management of moderate to severe acute pain and cancer pain, use of oxycodone imposes a risk of adverse effects such as addiction, overdose, and death. Fast and accurate determination of oxycodone blood concentration would enable personalized dosing and monitoring of the analgesic as well as quick diagnostics of possible overdose in emergency care. However, in addition to the parent drug, several metabolites are always present in the blood after a dose of oxycodone, and to date, there is no electrochemical data available on any of these metabolites. In this paper, a single-walled carbon nanotube (SWCNT) electrode and a Nafion-coated SWCNT electrode were used, for the first time, to study the electrochemical behavior of oxycodone and its two main metabolites, noroxycodone and oxymorphone. Both electrode types could selectively detect oxycodone in the presence of noroxycodone and oxymorphone. However, we have previously shown that addition of a Nafion coating on top of the SWCNT electrode is essential for direct measurements in complex biological matrices. Thus, the Nafion/SWCNT electrode was further characterized and used for measuring clinically relevant concentrations of oxycodone in buffer solution. The limit of detection for oxycodone with the Nafion/SWCNT sensor was 85 nM, and the linear range was 0.5-10 µM in buffer solution. This study shows that the fabricated Nafion/SWCNT sensor has potential to be applied in clinical concentration measurements.


Assuntos
Técnicas Eletroquímicas , Polímeros de Fluorcarboneto/química , Nanotubos de Carbono/química , Oxicodona/análise , Eletrodos , Estrutura Molecular , Oxicodona/metabolismo , Tamanho da Partícula , Propriedades de Superfície
11.
ACS Nano ; 14(4): 4298-4305, 2020 Apr 28.
Artigo em Inglês | MEDLINE | ID: mdl-32271541

RESUMO

Carbon nanotubes (CNTs) and boron nitride nanotubes (BNNTs) are one-dimensional materials with high thermal conductivity and similar crystal structures. Additionally, BNNTs feature higher thermal stability in air than CNTs. In this work, a single-walled carbon nanotube (SWCNT) film was used as a template to synthesize a BNNT coating by the chemical vapor deposition (CVD) method to form a coaxial heterostructure. Then, a contact-free steady-state infrared (IR) method was adopted to measure the in-plane sheet thermal conductance of the as-synthesized film. The heterostructured SWCNT-BNNT film demonstrates an enhanced sheet thermal conductance compared with the bare SWCNT film. The increase in sheet thermal conductance shows a reverse relationship with SWCNT film transparency. An enhancement of over 80% (from ∼3.6 to ∼6.4 µW·K-1·sq-1) is attained when the BNNT coating is applied to an SWCNT film with a transparency of 87%. This increase is achieved by BNNTs serving as an additional thermal conducting path. The relationship between the thermal conductance increase and transparency of the SWCNT film is studied by a structured modeling of the SWCNT film. We also discuss the effect of annealing on the thermal conductance of SWCNTs before BNNT growth. Along with the preservation of high electrical conductance, the enhanced thermal conductance of the heterostructured SWCNT-BNNT films makes them a promising building block for thermal and optoelectronic applications.

12.
Nano Lett ; 20(5): 3560-3567, 2020 May 13.
Artigo em Inglês | MEDLINE | ID: mdl-32324411

RESUMO

Heterostructures built from 2D, atomically thin crystals are bound by the van der Waals force and exhibit unique optoelectronic properties. Here, we report the structure, composition and optoelectronic properties of 1D van der Waals heterostructures comprising carbon nanotubes wrapped by atomically thin nanotubes of boron nitride and molybdenum disulfide (MoS2). The high quality of the composite was directly made evident on the atomic scale by transmission electron microscopy, and on the macroscopic scale by a study of the heterostructure's equilibrium and ultrafast optoelectronics. Ultrafast pump-probe spectroscopy across the visible and terahertz frequency ranges identified that, in the MoS2 nanotubes, excitons coexisted with a prominent population of free charges. The electron mobility was comparable to that found in high-quality atomically thin crystals. The high mobility of the MoS2 nanotubes highlights the potential of 1D van der Waals heterostructures for nanoscale optoelectronic devices.

13.
Science ; 367(6477): 537-542, 2020 01 31.
Artigo em Inglês | MEDLINE | ID: mdl-32001649

RESUMO

We present the experimental synthesis of one-dimensional (1D) van der Waals heterostructures, a class of materials where different atomic layers are coaxially stacked. We demonstrate the growth of single-crystal layers of hexagonal boron nitride (BN) and molybdenum disulfide (MoS2) crystals on single-walled carbon nanotubes (SWCNTs). For the latter, larger-diameter nanotubes that overcome strain effect were more readily synthesized. We also report a 5-nanometer-diameter heterostructure consisting of an inner SWCNT, a middle three-layer BN nanotube, and an outer MoS2 nanotube. Electron diffraction verifies that all shells in the heterostructures are single crystals. This work suggests that all of the materials in the current 2D library could be rolled into their 1D counterparts and a plethora of function-designable 1D heterostructures could be realized.

14.
ACS Omega ; 4(18): 17726-17734, 2019 Oct 29.
Artigo em Inglês | MEDLINE | ID: mdl-31681878

RESUMO

In clinical settings, the dosing and differential diagnosis of the poisoning of morphine (MO) and codeine (CO) is challenging due to interindividual variations in metabolism. However, direct electrochemical detection of these analytes from biological matrices is inherently challenging due to interference from large concentrations of anions, such as ascorbic acid (AA) and uric acid (UA), as well as fouling of the electrode by proteins. In this work, a disposable Nafion-coated single-walled carbon nanotube network (SWCNT) electrode was developed. We show facile electron transfer and efficient charge separation between the interfering anions and positively charged MO and CO, as well as significantly reduced matrix effect in human plasma. The Nafion coating alters the voltammetric response of MO and CO, enabling simultaneous detection. With this SWCNT/Nafion electrode, two linear ranges of 0.05-1 and 1-10 µM were found for MO and one linear range of 0.1-50 µM for CO. Moreover, the selective and simultaneous detection of MO and CO was achieved in large excess of AA and UA, as well as, for the first time, in unprocessed human plasma. The favorable properties of this electrode enabled measurements in plasma with only mild dilution and without the precipitation of proteins.

15.
J Am Chem Soc ; 141(42): 16553-16558, 2019 Oct 23.
Artigo em Inglês | MEDLINE | ID: mdl-31529952

RESUMO

High efficiency perovskite solar cells have underpinned the rapid growth of the field. However, their low device stability limits further advancement. Hygroscopic lithium bis(trifluoromethanesulfonyl)imide (Li+TFSI-) and metal electrode are the main causes of the device instability. In this work, the redox reaction between lithium-ion endohedral fullerenes and 2,2',7,7'-tetrakis(N,N-di-p-methoxyphenylamine)-9,9'-spirobi-fluorene (spiro-MeOTAD) was controlled to optimize the amount of oxidized spiro-MeOTAD and antioxidizing neutral endohedral fullerenes. Application of this mixture to metal-free carbon nanotube (CNT)-laminated perovskite solar cells resulted in 17.2% efficiency with a stability time of more than 1100 h under severe conditions (temperature = 60 °C, humidity = 70%). Such high performance is attributed to the uninhibited charge flow, no metal-ion migration, and the enhanced antioxidizing activity of the devices.

16.
ACS Nano ; 13(10): 11522-11529, 2019 Oct 22.
Artigo em Inglês | MEDLINE | ID: mdl-31497949

RESUMO

Transparent and conductive films (TCFs) are of great technological importance. Their high transmittance, electrical conductivity, and mechanical strength make single-walled carbon nanotubes (SWCNTs) a good candidate for the raw material for TCFs. Despite the ballistic transport in individual SWCNTs, electrical conductivity of SWCNT networks is limited by low efficiency of charge tunneling between the tube elements. Here, we demonstrate that the nanotube network sheet resistance at high optical transmittance is decreased by more than 50% when fabricated on graphene. This is a comparable improvement as that obtained through gold chloride (AuCl3) doping. However, while Raman spectroscopy reveals substantial changes in spectral features of AuCl3 doped nanotubes, this does not occur with graphene. Instead, temperature-dependent transport measurements indicate that a graphene substrate reduces the tunneling barrier heights, while its parallel conductivity contribution is almost negligible. Finally, we show that combining the graphene substrate and AuCl3 doping, brings the SWCNT thin film sheet resistance down to 36 Ω/□.

17.
J Phys Chem C Nanomater Interfaces ; 123(20): 13136-13140, 2019 May 23.
Artigo em Inglês | MEDLINE | ID: mdl-31156738

RESUMO

The chemical and electrical properties of single-walled carbon nanotubes (SWCNTs) and graphene can be modified by the presence of covalently bound impurities. Although this can be achieved by introducing chemical additives during synthesis, it often hinders growth and leads to limited crystallite size and quality. Here, through the simultaneous formation of vacancies with low-energy argon plasma and the thermal activation of adatom diffusion by laser irradiation, silicon impurities are incorporated into the lattice of both materials. After an exposure of ∼1 ion/nm2, we find Si-substitution densities of 0.15 nm-2 in graphene and 0.05 nm-2 in nanotubes, as revealed by atomically resolved scanning transmission electron microscopy. In good agreement with predictions of Ar irradiation effects in SWCNTs, we find Si incorporated in both mono- and divacancies, with ∼2/3 being of the first type. Controlled inclusion of impurities in the quasi-1D and -2D carbon lattices may prove useful for applications such as gas sensing, and a similar approach might also be used to substitute other elements with migration barriers lower than that of carbon.

18.
Opt Lett ; 44(7): 1750-1753, 2019 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-30933138

RESUMO

We develop a mode-locked Cr:ZnS polycrystalline laser using single-walled carbon nanotubes (SWCNTs) that have resonant absorption at the wavelength of 2.4 µm. The laser generates ultrashort pulses of 49 fs duration, a 2.4 µm center wavelength, and a 9.2 THz (176 nm) spectral span at a repetition rate of 76 MHz. We also confirm self-starting of the mode-locked operation. SWCNTs, if appropriately controlled in terms of their diameters, prove to be useful as ultrafast saturable absorbers in the mid-infrared region.

19.
Nano Lett ; 19(4): 2223-2230, 2019 04 10.
Artigo em Inglês | MEDLINE | ID: mdl-30517789

RESUMO

Single-walled carbon nanotubes (CNTs) has been considered as a promising material for a top electrode of perovskite solar cells owing to its hydrophobic nature, earth-abundance, and mechanical robustness. However, its poor conductivity, a shallow work function, and nonreflective nature have limited further enhancement in power conversion efficiency (PCE) of top CNT electrode-based perovskite solar cells. Here, we introduced a simple and scalable method to address these issues by utilizing an ex-situ vapor-assisted doping method. Trifluoromethanesulfonic acid (TFMS) vapor doping of the free-standing CNT sheet enabled tuning of conductivity and work function of the CNT electrode without damaging underneath layers. The sheet resistance of the CNT sheet was decreased by 21.3% with an increase in work function from 4.75 to 4.96 eV upon doping of TFMS. In addition, recently developed 2D perovskite-protected Cs-containing formamidium lead iodide (FACsPbI3) technology was employed to maximize the absorption. Because of the lowered resistance, better energy alignment, and improved absorption, the CNT electrode-based PSCs produced a PCE of 17.6% with a JSC of 24.21 mA/cm2, VOC of 1.005 V, and FF of 0.72. Furthermore, the resulting TFMS-doped CNT-PSCs demonstrated higher thermal and operational stability than bare CNT and metal electrode-based devices.

20.
ACS Nano ; 12(12): 11756-11784, 2018 12 26.
Artigo em Inglês | MEDLINE | ID: mdl-30516055

RESUMO

Advances in the synthesis and scalable manufacturing of single-walled carbon nanotubes (SWCNTs) remain critical to realizing many important commercial applications. Here we review recent breakthroughs in the synthesis of SWCNTs and highlight key ongoing research areas and challenges. A few key applications that capitalize on the properties of SWCNTs are also reviewed with respect to the recent synthesis breakthroughs and ways in which synthesis science can enable advances in these applications. While the primary focus of this review is on the science framework of SWCNT growth, we draw connections to mechanisms underlying the synthesis of other 1D and 2D materials such as boron nitride nanotubes and graphene.

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