Do carbon nanotubes catalyse bromine/bromide redox chemistry?
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ABSTRACT:
SUBMITTER: Kaliyaraj Selva Kumar A
PROVIDER: S-EPMC8372536 | biostudies-literature |
REPOSITORIES: biostudies-literature
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Project description:The strong affinity of carbon nanotubes (CNTs) to environmental contaminants has raised serious concern that CNTs may function as a carrier of environmental pollutants and lead to contamination in places where the environmental pollutants are not expected. However, this concern will not be realized until the contaminants are desorbed from CNTs. It is well recognized that the desorption of environmental pollutants from pre-laden CNTs varies with the environmental conditions, such as the solution pH and ionic strength. However, comprehensive investigation on the influence of solution chemistry on the desorption process has not been carried out, even though numerous investigations have been conducted to investigate the impact of solution chemistry on the adsorption of environmental pollutants on CNTs. The main objective of this study was to determine the influence of solution chemistry (e.g., pH, ionic strength) and surface functionalization on the desorption of preloaded 1,3,5-trichlorobenzene (1,3,5-TCB) from multi-walled carbon nanotubes (MWNTs). The results suggested that higher pH, ionic strength and natural organic matter in solution generally led to higher desorption of 1,3,5-TCB from MWNTs. However, the extent of change varied at different values of the tested parameters (e.g., pH < 7 vs. pH > 7). In addition, the impact of these parameters varied with MWNTs possessing different surface functional groups, suggesting that surface functionalization could considerably alter the environmental behaviors and impact of MWNTs.
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Project description:Carbon nanotubes (CNTs) possess remarkable mechanical, electrical, thermal, and optical properties that predestine them for numerous potential applications. The conventional chemical vapor deposition (CVD) route for the production of CNTs, however, suffers from costly and complex issues. Herein, we demonstrate a general and high-yield strategy to grow nitrogen-doped CNTs (NCNTs) on three-dimensional (3D) graphite felt (GF) substrates, through a direct thermal pyrolysis process simply using a common tube furnace, instead of the costly and complex CVD method. Specifically, the NCNTs-decorated GF (NCNT-GF) electrode possesses enhanced electrocatalytic performance towards cerium redox reactions, mainly due to the catalytic effect of N atoms doped into NCNTs, and ingenious and hierarchical 3D architecture of the NCNT-GF. As a result, the cell with the NCNT-GF serving as a positive electrode shows the improved energy efficiency with increases of about 53.4% and 43.8% over the pristine GF and the acidly treated GF at a high charge/discharge rate of 30 mA cm-2, respectively. Moreover, the as-prepared NCNT catalyst-enhanced electrode is found to be highly robust and should enable a long-term cycle without detectable efficiency loss after 500 cycles. The viable synthetic strategy reported in this study will contribute to the further development of more active heteroatom-doped CNTs for redox flow batteries.
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Project description:We demonstrate Ullmann-type reactions as novel and advantageous functionalization of carbon nanotubes (CNTs) toward tunable surface chemistry. The functionalization routes comprise O-, N-, and C-arylation of chlorinated CNTs. We confirm the versatility and efficiency of the reaction allowing functionalization degrees up to 3.5 mmol g-1 by applying both various nanotube substrates, i.e., single-wall (SWCNTs) and multi-wall CNTs (MWCNTs) of various chirality, geometry, and morphology as well as diverse Ullmann-type reagents: phenol, aniline, and iodobenzene. The reactivity of nanotubes was correlatable with the nanotube diameter and morphology revealing SWCNTs as the most reactive representatives. We have determined the optimized conditions of this two-step synthetic protocol as: (1) chlorination using iodine trichloride (ICl3), and (2) Ullmann-type reaction in the presence of: copper(I) iodide (CuI), 1,10-phenanthroline as chelating agent and caesium carbonate (Cs2CO3) as base. We have analyzed functionalized CNTs using a variety of techniques, i.e., scanning and transmission electron microscopy, energy dispersive spectroscopy, thermogravimetry, comprehensive Raman spectroscopy, and X-ray photoelectron spectroscopy. The analyses confirmed the purely covalent nature of those modifications at all stages. Eventually, we have proved the elaborated protocol as exceptionally tunable since it enabled us: (a) to synthesize superhydrophilic films from-the intrinsically hydrophobic-vertically aligned MWCNT arrays and (b) to produce printable highly electroconductive pastes of enhanced characteristics-as compared for non-modified and otherwise modified MWCNTs-for textronics.
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Project description:In this paper we report the first observation, through X-ray diffraction, of noncovalent uracil-uracil (U-U) dimeric ?-stacking interactions in carbon nanotube (CNT)-based supramolecular assemblies. The directionally oriented morphology determined using atomic force microscopy revealed highly organized behavior through ?-stacking of U moieties in a U-functionalized CNT derivative (CNT-U). We developed a dispersion system to investigate the bio-inspired interactions between an adenine (A)-terminated poly(3-adeninehexyl thiophene) (PAT) and CNT-U. These hybrid CNT-U/PAT materials interacted through ?-stacking and multiple hydrogen bonding between the U moieties of CNT-U and the A moieties of PAT. Most importantly, the U···A multiple hydrogen bonding interactions between CNT-U and PAT enhanced the dispersion of CNT-U in a high-polarity solvent (DMSO). The morphology of these hybrids, determined using transmission electron microscopy, featured grape-like PAT bundles wrapped around the CNT-U surface; this tight connection was responsible for the enhanced dispersion of CNT-U in DMSO.
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Project description:Graphitic carbons have been used as conductive supports for developing rechargeable batteries. However, the classic ion intercalation in graphitic carbon has yet to be coupled with extrinsic redox reactions to develop rechargeable batteries. Herein, we demonstrate the preparation of a free-standing, flexible nitrogen and phosphorus co-doped hierarchically porous graphitic carbon for iodine loading by pyrolysis of polyaniline coated cellulose wiper. We find that heteroatoms could provide additional defect sites for encapsulating iodine while the porous carbon skeleton facilitates redox reactions of iodine and ion intercalation. The combination of ion intercalation with redox reactions of iodine allows for developing rechargeable iodine-carbon batteries free from the unsafe lithium/sodium metals, and hence eliminates the long-standing safety issue. The unique architecture of the hierarchically porous graphitic carbon with heteroatom doping not only provides suitable spaces for both iodine encapsulation and cation intercalation but also generates efficient electronic and ionic transport pathways, thus leading to enhanced performance.Carbon-based electrodes able to intercalate Li+ and Na+ ions have been exploited for high performing energy storage devices. Here, the authors combine the ion intercalation properties of porous graphitic carbons with the redox chemistry of iodine to produce iodine-carbon batteries with high reversible capacities.
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Project description:We describe the preparation of hybrid redox materials based on polyoxomolybdates encapsulated within single-walled carbon nanotubes (SWNTs). Polyoxomolybdates readily oxidize SWNTs under ambient conditions in solution, and here we study their charge-transfer interactions with SWNTs to provide detailed mechanistic insights into the redox-driven encapsulation of these and similar nanoclusters. We are able to correlate the relative redox potentials of the encapsulated clusters with the level of SWNT oxidation in the resultant hybrid materials and use this to show that precise redox tuning is a necessary requirement for successful encapsulation. The host-guest redox materials described here exhibit exceptional electrochemical stability, retaining up to 86 % of their charge capacity over 1000 oxidation/reduction cycles, despite the typical lability and solution-phase electrochemical instability of the polyoxomolybdates we have explored. Our findings illustrate the broad applicability of the redox-driven encapsulation approach to the design and fabrication of tunable, highly conductive, ultra-stable nanoconfined energy materials.
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