Dataset Information

Probing Mechanistic Insights into Highly Efficient Lithium Storage of C₆₀ Fullerene Enabled via Three-Electron-Redox Chemistry.

ABSTRACT: Renewable organic cathodes with abundant elements show promise for sustainable rechargeable batteries. Herein, for the first time, utilizing C₆₀ fullerene as organic cathode for room-temperature lithium-ion battery is reported. The C₆₀ cathode shows robust electrochemical performance preferably in ether-based electrolyte. It delivers discharge capacity up to 120 mAh g^-1 and specific energy exceeding 200 Wh kg^-1 with high initial Coulombic efficiency of 91%. The as-fabricated battery holds a capacity of 90 mAh g^-1 after 50 cycles and showcases remarkable rate performance with 77 mAh g^-1 retained at 500 mA g^-1 . Noteworthily, three couples of unusual flat voltage plateaus recur at ≈2.4, 1.7, and 1.5 V, respectively. Diffusion-dominated three-electron-redox reactions are revealed by cyclic voltammogram and plateau capacities. Intriguingly, it is for the first time unveiled by in situ X-ray diffraction (XRD) that the C₆₀ cathode underwent three reversible phase transitions during lithiation/delithiation process, except for the initial discharge when irreversible polymerization in between C₆₀ nanoclusters existed as suggested by the characteristic irreversible peak shifts in both in situ XRD pattern and in situ Raman spectra. Cs-corrected transmission electron microscope corroborated these phase evolutions. Importantly, delithiation potentials derived from density-functional-theory simulation based on proposed phase structures qualitatively consists with experimental ones.

SUBMITTER: Qiu H

PROVIDER: S-EPMC8425916 | biostudies-literature | 2021 Sep

REPOSITORIES: biostudies-literature

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Probing Mechanistic Insights into Highly Efficient Lithium Storage of C60 Fullerene Enabled via Three-Electron-Redox Chemistry.

Qiu Haifa H Wan Jing J Zhang Junxian J Wang Xin X Zhang Nianji N Chen Rouxi R Xia Yu Y Huang Li L Wang Hsing-Lin HL

Advanced science (Weinheim, Baden-Wurttemberg, Germany) 20210711 17

Renewable organic cathodes with abundant elements show promise for sustainable rechargeable batteries. Herein, for the first time, utilizing C60 fullerene as organic cathode for room-temperature lithium-ion battery is reported. The C60 cathode shows robust electrochemical performance preferably in ether-based electrolyte. It delivers discharge capacity up to 120 mAh g-1 and specific energy exceeding 200 Wh kg-1 with high initial Coulombic efficiency o ...[more]

PMID: 34250756

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Project description:The photodynamic action mechanism sensitized by a non-charged porphyrin-fullerene C60 dyad (TCP-C60) and its tetracationic analogue (TCP-C60 4+) was investigated in solution and in Staphylococcus aureus cells. The ability of both dyads to form a photoinduced charge-separated state was evidenced by the reduction of methyl viologen in N,N-dimethylformamide (DMF). Moreover, the formation of superoxide anion radicals induced by these dyads was detected by the reduction of nitro blue tetrazolium. Also, photosensitized decomposition of l-tryptophan (Trp) was investigated in the presence of reactive oxygen species (ROS) scavengers. The addition of β-carotene and sodium azide had a slight effect on reaction rate. However, photooxidation of Trp mediated by TCP-C60 was negligible in the presence of d-mannitol, while no protection was found using TCP-C60 4+. In a polar medium, these dyads mainly act by a contribution of type I pathway with low generation of singlet molecular oxygen, O2(1Δg). In S. aureus cell suspensions, an aerobic atmosphere was required for the photokilling of this bacterium. The photocytotoxicity induced by TCP-C60 was increased in D2O with respect to water, while a small effect was found using TCP-C60 4+. Furthermore, photoinactivation of microbial cells was negligible in the presence of sodium azide. The addition of d-mannitol did not affect the photoinactivation induced by TCP-C60. In contrast, S. aureus cells were protected by d-mannitol when TCP-C60 4+ was used as a photosensitizer. Also, generation of O2(1Δg) in the S. aureus cells was higher for TCP-C60 than TCP-C60 4+. Therefore, TCP-C60 appears to act in microbial cells mainly through the mediation of O2(1Δg). Although, a contribution of the type I mechanism was found for cell death induced by TCP-C60 4+. Therefore, these dyads with high capacity to produce photoinduced charge-separated state represent interesting photosensitizers to inactivate microorganisms by type I or type II mechanisms. In particular, TCP-C60 may be located in a non-polar microenvironment in the cells favoring a type II pathway, while a contribution of the type I mechanism was produced using the cationic TCP-C60 4+.

Project description:The human body contains 60-70% water, depending on age. As a body fluid, it is not only a medium in which physical and chemical processes take place, but it is also one of the active mediators. Water is the richest substance with non-covalent hydrogen bonds. Water molecules, by themselves (in vacuum), are diamagnetic but when organized into clusters, they become diamagnetic or paramagnetic. Also, biomolecules (DNA, collagen, clathrin, and other proteins) have non-covalent hydrogen bonds in their structure. The interaction, as well as signal transmission, between water and biomolecules is achieved through the vibrations of covalent and non-covalent hydrogen bonds, which determine the state and dynamics of conformational changes in biomolecules. Disruptive conformational changes in biomolecules, cells, and tissues lead to their dysfunctionality, so they are a frequent cause of many disorders and diseases. For example, the rearrangement of hydrogen bonding due to mitochondrial disease mutation in cytochrome bc1 disturbs heme bH redox potential and spin state. In order to prevent and repair the dysfunctional conformational changes, a liquid substance was developed based on the second derivative of the C60 molecule (SD-C60), which has classical and quantum properties. The characterization of SD-C60 by UV-VIS-NIR, FTIR, TEM, and AFM/MFM was performed and it is shown that SD-C60 water layers generate vibrations with near-zero phase dispersion which are transmitted through Fibonacci's water chains to biomolecules. In comparison with previously published SD-C60 derivate (3HFWC, size until 10 nm, and 1-5 water layers), the improved formulation (3HFWC-W, size 10-25 nm, and 6-9 water layers) showed multiplied cytotoxic activity against melanoma cell lines of different aggressiveness. Apart from this, the mode of action was preserved and based on an induction of senescence rather than cell death. Importantly, high selectivity towards malignant phenotypes was detected. Observed effects can be ascribed to a machinery of hydrogen bonds, which are generated in SD-C60 and transmitted through water to biomolecules. This approach may open a new field in science and healthcare-a "water-based nanomedicine".

Project description:A photostable and photodynamic antimicrobial surface was successfully obtained and applied to photoinactivate microorganisms. This approach was based on the synthesis of a fullerene C60 derivative (EDOT-C60) where fullerene C60 is covalently linked to 3,4-ethylenedioxythiophene (EDOT) through a 1,3-dipolar cycloaddition reaction. This dual-functional monomer bears an EDOT center connected via an alkyl chain to a fullerene C60 moiety. In this structure, EDOT acts as an electropolymerizable unit that allows the film formation over conducting substrates, while fullerene C60 performs the photodynamic antimicrobial activity. Electrochemical polymerization of EDOT was used to obtain stable and photodynamic polymeric films (PEDOT-C60) in a controllable procedure. Cyclic voltammetry and UV-visible spectroscopy studies showed that the fullerene C60 units were not altered during the electropolymerization process, obtaining surfaces with high fullerene content. Photobleaching measurements demonstrated that the electropolymerized films were highly photostable. Moreover, photodynamic properties of PEDOT-C60 were compared with fullerene C60 and showed that electrodeposited films were able to generate reactive oxygen species (ROS) through the two photomechanisms, producing singlet molecular oxygen (type II) and superoxide radical anion (type I). All studies demonstrated that fullerene C60 moieties covalently attached to the polymeric matrix mainly conserve the photodynamic characteristics. Hence, photodynamic action sensitized by PEDOT-C60 was assessed in vitro against Staphylococcus aureus. The photosensitized inactivation by the electropolymerized films on bacteria suspensions produced >99.9% reduction in S. aureus survival. Fluorescence microscopy experiments with S. aureus adhered to the PEDOT-C60 surface showed a complete microbe annihilation. Also, the eradication of biofilms formed on PEDOT-C60 surfaces resulted in a photokilling >99.9% after visible light irradiation. Our results demonstrated that these antimicrobial photodynamic polymeric films are a promising and versatile platform to photoinactivate microorganisms and to obtain photostable self-sterilizing surfaces.

Dataset Information

Probing Mechanistic Insights into Highly Efficient Lithium Storage of C₆₀ Fullerene Enabled via Three-Electron-Redox Chemistry.

Publications

Probing Mechanistic Insights into Highly Efficient Lithium Storage of C<sub>60</sub> Fullerene Enabled via Three-Electron-Redox Chemistry.

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