Carbon nanotubes (CNTs) are materials with exceptional electrical, thermal, mechanical, and optical properties. Ever since it was demonstrated that they also possess interesting thermoelectric properties, they have been considered a promising solution for thermal energy harvesting. In this study, we present a simple method to enhance their performance. For this purpose, thin films obtained from high-quality single-walled CNTs (SWCNTs) were doped with a spectrum of inorganic and organic halide compounds. We studied how incorporating various halide species affects the electrical conductivity, the Seebeck coefficient, and the Power Factor. Since thermoelectric devices operate under non-ambient conditions, we also evaluated these materials' performance at elevated temperatures. Our research shows that appropriate dopant selection can result in almost fivefold improvement to the Power Factor compared to the pristine material. We also demonstrate that the chemical potential of the starting CNT network determines its properties, which is important for deciphering the true impact of chemical and physical functionalization of such ensembles.

We report on the development of a method of formation of hydrophilic carbon nanotube (CNT) films. The technique is simple, straightforward and does not require specialized equipment or use of harsh chemical compounds. Elimination of the need for oxidizing agents has paramount implications because it preserves the inherent CNT properties. A reference study, in which the traditional method of oxidation of CNTs was used to introduce functional groups, gave smaller reduction of water contact angle and made a negative influence on the surface chemistry. From the practical point of view, this method is an important step towards implementation of CNTs in the real life by making them more compatible with interface materials. Interestingly, the method gives high level of control over the surface character of CNT films and hydrophilic character can be precisely patterned where required.

Despite the widespread use of sonication for individualization of nanomaterials, its destructive nature is rarely acknowledged. In this study, we demonstrated how exposure of the material to a hostile sound wave environment can be limited by the application of another preprocessing step. Single-walled carbon nanotubes (CNTs) were initially ground in a household coffee grinder, which enabled facile deagglomeration thereof. Such a simple approach enabled us to obtain high-quality CNT dispersion at reduced sonication time. Most importantly, electrical conductivity of free-standing films prepared from these dispersion was improved almost fourfold as compared with unground material eventually reaching 1067 ± 34 S/cm. This work presents a new approach as to how electrical properties of nanocarbon ensembles may be enhanced without the application of doping agents, the presence of which is often ephemeral.

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Metrics & MoreArticle Recommendations CONSPECTUS:The surface of 2D materials can spontaneously adsorb and react with molecules in the environment during their processing and storage. This effect, while having a significant impact on many properties of 2D materials, is not always recognized and accounted for in the research involving them. This Account summarizes our recent work in understanding how the ambient environment impacts the properties of 2D materials and its mitigation strategies. We highlight graphene and hydrocarbons in our discussion and complement it with selected studies involving other 2D materials as well as water and oxygen.When graphene and graphite are exposed to air and water, their surfaces adsorb the residue hydrocarbons, typically at part-pertrillion to part-per-billion levels, in the environment. The adsorption of hydrocarbons reduces the surface energy of graphene and graphite and creates a barrier between them and the electrolyte. As a result, the wettability and electrochemical properties of graphene and graphite can be significantly altered by mere exposure to the ambient environment. These changes can be very significant yet highly variable depending on the local environment: several hours of air exposure can increase the water contact angle of graphene by up to 40°and reduce the double-layer capacitance of graphite by up to 50%! The high hydrophobicity and poor electrochemical performance of pristine graphitic carbons, once believed to be intrinsic properties of these materials, are largely due to unintentional surface contamination. The same type of hydrocarbon adsorption was reported for many other 2D materials, such as MoS 2 , hexagonal BN, and mica. In the case of mica, which is highly ionic in nature, the adsorption of hydrocarbons disrupts its interaction with ionic liquid and alters the self-assembly structure of ionic liquid at the mica surface. Similarly, water also impacts the surface properties of graphene in several ways. Water vapor can compete with hydrocarbons for adsorption onto the surface of graphene, thus reducing the rate of hydrocarbon contamination. Water can intercalate between graphene and some of its supporting substrate, altering their interactions. Finally, water enhances the doping of 2D materials by O 2 by promoting an electrochemical doping mechanism involving the O 2 /H 2 O redox couple.Reducing and reversing the surface contamination of 2D materials can greatly enhance material and device performances. While completely stopping the contamination is still challenging, a high-humidity environment is shown to reduce the rate of contamination, as mentioned above. For samples already contaminated by airborne hydrocarbons, their surface properties can be partially restored by treatment in high-vacuum, high-temperature, or mildly oxidative environments.

Partial oxidation of nanocarbon materials is one of the most straightforward methods to improve their compatibility with other materials, which widens its application potential. This work studied how the microstructure and properties of high crystallinity single-walled carbon nanotubes (SWCNTs) can be tailored by applying the modified Hummers method. The influence of temperature (0, 18, 40 °C), reaction time (0 min to 7 h), and the amount of KMnO4 oxidant was monitored. The results showed that depending on the oxidation conditions, the electronic characteristics of the material could be adjusted. After optimizing the parameters, the SWCNTs were much more conductive (1369 ± 84 S/cm with respect to 283 ± 32 S/cm for the untreated material). At the same time, the films made from them exhibited hydrophilic character of the surface (water contact angle changed from 71° to 27°).

We have demonstrated that large diameter (1.8 ± 0.4 nm) carbon nanotubes (CNTs) can be separated by means of the aqueous two-phase extraction (ATPE). This rapid and convenient tool has enabled us to isolate fractions of particular CNT diameter distribution. We have shown how a range of parameters can be used to fine tune the characteristics of the isolated material. Interestingly, by varying the pH of the medium, we have suppressed the extraction of low diameter CNTs and only large diameter CNTs were obtained. A number of other factors such as selected surfactant concentration steps, temperature or amount of starting CNT material have been found to have a significant effect on the end result of the CNT differentiation. The findings have provided us with more insight regarding the underlying mechanics of ATPE for processing polydisperse CNT mixtures.