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Medium-temperature fluoroalkylation of microporous activated carbons (ACs) with 1,1,1,2-tetrafluoroethane is presented. Supercapacitor (SC) electrodes based on the fluoroalkylated ACs showed enhanced specific capacitance and high specific energy in electrolytes, either aqueous potassium hydroxide solution or tetraethylammonium tetrafluoroborate-acetonitrile solution. We found the largest increase in the specific capacitance, up to 89 F g–1, and in the specific energy, up to 7.5 Wh kg–1, at the voltage of 1.5 V. The specific capacitance of the SC electrode based on the sample prepared at 350 °C increases by a factor of ~ 2–3 × for certain scan rates in the organic electrolyte. The fluoroalkylated ACs have good electrochemical stability in the tested model systems. We associate the registered enhanced SC parameters with an increase in the total fluorine content and high specific surface areas of the carbon electrode materials. The surface “isolated fluorine” formed during fluoroalkylation at 300–400 °C ensures the production of improved electrode materials for SC applications. Fluoroalkylation is a simple and cost-effective method of improving the specific capacitance of carbon-based SC electrodes.

Surface decoration of graphene-based nanostructures with metals has been predicted to be an efficient way towards the development of resistant catalysts and novel materials for energy applications, such as hydrogen production and storage. We report on an extensive neutron scattering study of a defective graphene-based material decorated with nickel nanoparticles, obtained via the chemical decoration of thermally exfoliated graphite oxide. The combination of neutron diffraction and inelastic neutron scattering measurements has been used to characterize the low-dimensional carbon backbone and the presence of the nickel nanoparticles, organized at the nanometer scale on the graphene plane. The structural features of this system, along with the nickel capability of dissociating the hydrogen molecule upon hydrogen treatment, are herein discussed.

Graphene-based miniaturized supercapacitors, obtained via laser conversion of suitable precursors, have been attracting recent attention for the production of energy storage small-scale devices. In this work, a one-pot synthesis of TiO2 nanoparticles embedded in porous graphene-based electrodes has been obtained with the LightScribe® technology, by converting the precursor materials through the absorption of a DVD burner infrared laser light. Enhanced electrochemical performance of devices has been achieved thanks to the combination of faradic surface reactions, arising from metal oxide nanoparticles, with the conventional electrochemical double layer capacitance, arising from porous graphene. Micro-supercapacitors, consisting of TiO2-graphene electrodes, have been tested by investigating two hydrogel polymer electrolytes, based on polyvinyl alcohol/H3PO4 and polyvinyl alcohol/H2SO4, respectively. Specific areal capacitance up to 9.9 mF/cm2 are obtained in TiO2-graphene devices, corresponding to a volumetric capacitance of 13 F/cm3 and doubling the pristine graphene-based device results. The micro-supercapacitors achieved specific areal energy and specific areal power of 0.22 μWh/cm2 and 39 μW/cm2, along with a cyclability greater than 3000 cycles. These high-performance results suggest laser-scribed TiO2-graphene nanostructures as remarkable candidates in micro-supercapacitors for environment-friendly, large-scale and low-cost applications.

Oxidation of activated carbon (AC) with nitric acid was carried out, and the resulting AC/HNO 3 showed high capacity when used as supercapacitor electrode material operated in the KOH electrolyte. Oxidation caused different structural changes in the AC, reducing the specific surface area and the total pore volume. After oxidation, the content of all types of oxygen-containing groups and, especially, carboxyl groups showed a significant increase. Despite the significant reduction of the specific surface area, the specific capacitance of the oxidized AC in symmetric supercapacitor electrodes is 1.4 times larger than that for the pristine AC.

Optical excitation at terahertz frequencies has emerged as an effective means to manipulate complex solids dynamically. In the molecular solid K3C60, coherent excitation of intramolecular vibrations was shown to transform the high temperature metal into a non-equilibrium state with the optical conductivity of a superconductor. Here we tune this effect with hydrostatic pressure, and we find it to disappear around 0.3 GPa. Reduction with pressure underscores the similarity with the equilibrium superconducting phase of K3C60, in which a larger electronic bandwidth is detrimental for pairing. Crucially, our observation excludes alternative interpretations based on a high-mobility metallic phase. The pressure dependence also suggests that transient, incipient superconductivity occurs far above the 150 K hypothesised previously, and rather extends all the way to room temperature., 33 pages, 17 figures, 2 tables

We report on the C-60, Na, and Li dynamics in NaxLi6xC60 fullerides (x = 0, 1, 5, and 6) in the temperature range 80-550 K by using C-13, Na-23, and Li-7 solid state NMR. The results show that the C-60 reorientation dynamics is hindered at room temperature for the Li-enriched fullerides, but it is active for the Na rich ones with a rate of the order of few kilohertz. Na-23 and Li-7 NMR measurements show the presence of two dominant thermally activated dynamics that can be associated with Li/Na ionic motions within the octahedral sites (intrasite motion) and between the octahedral and tetrahedral sites (intersite motion). The substitution of one Na or one Li ion in the end members Li6C60 and Na6C60, respectively, yields to an increase of the hopping rate of the intersite motion, which is necessary for the ionic diffusion in possible fulleride-based ionic conductors.

Having single atoms or small clusters docked onto a single layer graphene represents a charming feature for energy-storage and catalysis. Unfortunately, the large cohesion energy of transition metals often prevents the isolation of nanoscopic clusters, which invariably tend to aggregate. The decoration of defective graphene layers with single Pt atoms and sub-nanometric clusters is herein achieved by exploiting metal carbonyl clusters, as precursor, and investigated by means of transmission electron microscopy and X-ray photoemission spectroscopy. Unexpectedly, the process of aggregation of Pt into larger clusters is inhibited onto the surface of defective graphene, where the Pt-clusters are found to fragment even into single metal atoms.

The addition of transition metals to alkali intercalated fullerides proved to enhance their already good hydrogen absorption properties. Herein we present a study based on two different synthetic strategies, allowing the addition of nickel as aggregates with different size to the lithium fulleride Li6C60: the former is based on the metathesis of nickel chloride, while the latter on the thermal decomposition of nickel carbonyl clusters. The hydrogen-storage properties of the obtained materials have been investigated with manometric and calorimetric measurements, which indicated a clear enhancement of the final absorption value and kinetics with respect to pristine Li6C60, as a consequence of nickel surface catalytic activity towards hydrogen molecules dissociation. We found up to 10 % increase of the total H2 weight % absorbed (5.5 wt% H2) in presence of Ni aggregates. Furthermore, the control of the transition metal particles size distribution allowed reducing the hydrogen desorption enthalpy of the systems.

The applicability of Cu/C catalysts is limited by sintering of Cu leading to deactivation in catalytic reactions. We show that the problem of sintering could be resolved by N-doping of the carbon support. Cu nanocatalysts with 1 at% of metal were synthesized by Cu acetate decomposition on N-free and N-doped (5.7 at% N) mesoporous carbon supports as well as on thermally expanded graphite oxide. Catalytic properties of these samples were compared in hydrogen production from formic acid decomposition. The N-doping leads to a strong interaction of the Cu species with the support providing stabilization of Cu in the form of clusters of less than 5 nm in size and single Cu atoms, which were observed in a significant ratio by atomic resolution HAADF/STEM even after testing the catalyst under harsh conditions of the reaction at 600 K. The mean size of the obtained Cu clusters was by a factor of 7 smaller than that of the particles in the N-free catalyst. The N-doped Cu catalyst possessed good stability in the formic acid decomposition at 478 K for at least 7 h on-stream and a significantly higher catalytic activity than the N-free Cu catalysts. The nature of the strongly interacting Cu species was studied by XPS, XRD and other methods as well as by DFT calculations. The presence of single Cu atoms in the N-doped catalysts should be attributed to their strong coordination by pyridinic nitrogen atoms at the edge of the graphene sheets of the support. We believe that the N-doping of the carbon support will allow expanding the use of Cu/C materials for different applications avoiding sintering and deactivation.

Melanophlogite (type I clathrate) has a microporous framework of corner sharing SiO4 tetrahedra, which can host guest gases. Here, a multi–analytical approach has been employed to understand the phase transitions with temperature and the degassing behaviour of a melanophlogite sample, which contains CO2 together with minor CH4 amount as enclathrated molecules.Synchrotron powder diffraction data collected between 110 and 380 K (ESRF, ID22 beamline) show a clear splitting of the major peaks up to about 360 K. Le Bail analysis shows that the low temperature phase is monoclinic, changing to cubic at ∼370 K. Landau theory analysis indicates that the transition is second order, with Tc = 369(1) K. Moreover, significant volume strain related to the phase transitions accounts for the lower thermal expansion at higher temperature. Differential scanning calorimetry shows evidence of a further phase transition between 220 and 250 K. The transition is confirmed by powder diffraction, with a change in slope in the b unit cell parameter and in volume expansion in the same temperature range. High temperature X-Ray powder diffraction between 313 and 673 K shows that thermal expansion decreases with temperature, possibly in relation with a structural rearrangement within the cubic structure during degassing. Thermogravimetric analysis shows that degassing of the guest gases begins at 450 K, and occurs at a higher rate above 750 K, but it is not completed even at T = 1273 K. Melanophlogite confirms to be a good host carrier for the gases, with gas loss only at higher temperature. Moreover, as degassing occurs with almost no thermal expansion, it could open promising application for its mechanical stability during degassing.

We report on the preparation of a novel hierarchically-porous super-activated carbon originating from organic waste with specific surface area exceeding 3000 m2/g, obtained starting from biochar derived by the pyrolysis of poultry litter. The chemical activation process proved to be efficient to remove the majority of impurities other than carbon, stabilizing a highly porous hierarchical structure with local graphene-like morphology. The presence of P and S with concentration below 0.1 wt% distinguishes this activated carbon from the usual ones obtained from vegetal sources. Thanks to these features, the obtained porous compound demonstrated to behave as an excellent electrode material for high-performance symmetric supercapacitors, reaching high specific capacitance up to 229 (13) F/g. Remarkably, the devices also supply high current density of 10 A/g without using any conducting additives and display high power density and reliability. Moreover, these optimal performances have been obtained operating by using simple eco-friendly electrolytes, like KOH and Na2SO4 aqueous solutions. The availability, the biocompatibility and the inexpensiveness of the starting materials, together with the low environmental impact of the electrolyte, suggest possible large-scale applications for such devices, for example in the field of transportation or in renewable energy-grids, but also in the field of bio-medicine.

The lithium cluster intercalated fulleride Li 12 C 60 was investigated by means of Muon Spin Relaxation (μSR) spectroscopy with the intent of unveil its hydrogen storage mechanism. Thanks to the well-known propensity of positive muons to form Muonium, a light isotope of the hydrogen atom, the final stages of the absorption process can be probed. The appearance of a slow oscillating signal in the time evolution of the muon polarization indicates the presence of Li–Mu covalent pair, never observed before in lower doped Li fullerides, which mimics the formation of LiH at the first stage of hydrogen chemisorption in the material. In addition, the μSR signal shows a clear transition above 150 K, compatible with a thermally activated Li cluster rearrangement. The combined Inelastic Neutron Scattering analysis suggests that tetrahedral Li clusters may undergo a progressive melting upon heating, which could favour room temperature ionic diffusion.

We herein report on the synthesis of mixed alkali cluster intercalated fullerides NaxLiy−xC60 (y = 12; x = 1–6) by a two-steps mechanochemical reaction of fullerene with sodium and lithium. These compounds crystallize in the cubic lattice of C60 displaying a contracted lattice parameter with respect to the Na6C60 parent structure. The analysis of the hydrogen sorption behaviour shows a slight decrease in the dehydrogenation enthalpy for y = 12 with respect to the sodium free member. Raman spectroscopy highlighted a partial electron transfer from alkali metals to C60, suggesting the presence of charged sodium/lithium clusters. Finally, we applied muon spectroscopy to understand the different hydrogenation mechanisms in NaxLi6−xC60 and NaxLi12−xC60 and explain their different performance.

Li6C60 has been chosen as the most representative system to study the hydrogenation mechanism in alkali-cluster intercalated fullerides. We present here a muon spin relaxation (mu SR) experiment that hints the chance to achieve a higher storage capacity on fullerene with respect to the values suggested in literature. Moreover, a linear relationship between the muonium adduct radical hyperfine frequency and the level of C-60 hydrogenation was found and it can be exploited to probe the C-60 hydrogenation level, giving more credit to this technique in the field of hydrogen storage materials. (C) 2017 Elsevier Ltd. All rights reserved.

After the successful electrochemical intercalation of C 60 with sodium, we report here the preparation of novel negative electrodes for Na-ion batteries composed by commercial C 60 :C 70 mixture, this being significantly less expensive than pure fullerenes. An optimized solid-state Na-poly(ethylene oxide) electrolyte was used for the battery assembly. While pure C 60 electrodes show a strong irreversible behavior after the first discharge, the peculiar disordered crystalline arrangement of C 60 and C 70 in the mixture, increased by a high-energy ball milling treatment, allows to improve the specific capacity at the first discharge up to 320 mAh/g, as well as the overall reversibility.

The lithium-intercalated fulleride Li12C60 was investigated in view of a lightweight hydrogen storage material due to the low molecular weight of its constituents. Deuterium (D2) absorption in Li12C60 shows an uptake of up to 9.5 mass % D2 (equivalent to ∼5 mass % H2 for the same stoichiometry). Under a pressure of 190 bar the onset of absorption was observed at a temperature below 100 C, which is 200 C lower than that for pure C60. Deuterium desorption was investigated by in-situ neutron powder diffraction, and at a pressure of 1 bar desorption was observed above 300 C. The ab/desorption is accompanied by a partial de/reintercalation of lithium, observed by the appearance and disappearance of LiD reflections after absorption and during desorption, respectively. A minor part of deuterium is present in ionic form in LiD, and the major part is covalently bound in a Li-depleted compound Li 12-xC60D36+y. © 2013 American Chemical Society.

Single-walled carbon nanotubes (SWCNTs) possessing a confined inner space protected by chemically resistant shells are promising for delivery, storage, and desorption of various compounds, as well as carrying out specific reactions. Here, we show that SWCNTs interact with molten mercury dichloride (HgCl2) and guide its transformation into dimercury dichloride (Hg2Cl2) in the cavity. The chemical state of host SWCNTs remains almost unchanged except for a small p-doping from the guest Hg2Cl2 nanocrystals. The density functional theory calculations reveal that the encapsulated HgCl2 molecules become negatively charged and start interacting via chlorine bridges when local concentration increases. This reduces the bonding strength in HgCl2, which facilitates removal of chlorine, finally leading to formation of Hg2Cl2 species. The present work demonstrates that SWCNTs not only serve as a template for growing nanocrystals but also behave as an electron-transfer catalyst in the spatially confined redox reaction by donation of electron density for temporary use by the guests.

Lithium and hydrogen dynamics in Li12C60 and Li12C60Hy are investigated by means of 7Li and 1H solid state Nuclear Magnetic Resonance (NMR) in the temperature range 80–550 K. Differential scanning calorimetry characterization on the hydrogen sorption and X-rays structural analysis are also reported. In the pure phase, the 7Li results show a thermally activated dynamics that can be associated to Li motions within the crystal interstices. Upon hydrogenation, Li ionic motion is considerably hindered by the presence of hydrofullerene molecules. The 1H measurements show that C–H bonds are stable on the local scale up to 400–450 K. The NMR results at higher temperatures are compatible with a H diffusion mechanism which anticipates the H desorption process.

Through the substitution of Li with Na in Li6C60, we synthesized a series of mixed alkali cluster intercalated fullerides, NaxLi6−xC60. These compounds share lattices of Na6C60 and Li6C60 with a cubic parameter linearly dependent on x. H2 absorption and desorption were studied by means of charge/discharge kinetic measurements and coupled calorimetric–manometric evaluation. By varying the stoichiometry, we found the best compromise among the absorption rate, temperature and amount of hydrogen for x = 0.5 and 1. Small concentrations of Na substituted to Li significantly lower the absorption temperature of Li6C60, improving the hydrogenation capacity, the kinetics, and the dehydrogenation enthalpy, the latter being 43.8 kJ mol−1 H2 for x = 1. This study moves further toward the utilization of intercalated fullerides for hydrogen storage applications.

Two chemically synthesized defective graphene materials with distinctly contrasting extended structures and surface chemistry are used to prepare sodium-ion battery electrodes. The difference in electrode performance between the chemically prepared graphene materials is qualified based on correlations with intrinsic structural and chemical dissimilarities. The overall effects of the materials’ physical and chemical discrepancies are quantified by measuring the electrode capacities after repeated charge/discharge cycles. Solvothermal synthesized graphene (STSG) electrodes produce capacities of 92 mAh/g in sodium-ion batteries after 50 cycles at 10 mA/g, while thermally exfoliated graphite oxide (TEGO) electrodes produce capacities of 248 mAh/g after 50 cycles at 100 mA/g. Solid-state 23Na nuclear magnetic resonance spectroscopy is employed to locally probe distinct sodium environments on and between the surface of the graphene layers after charge/discharge cycles that are responsible for the variations in ...

The hydrogen absorption of sodium intercalated fullerenes (Na xC60) was determined and compared to pure fullerenes (C60). Up to 3.5 mass% hydrogen can reversibly be absorbed in Na xC60 at 200 °C and a hydrogen pressure of 200 bar. The absorbed amount of hydrogen is significantly higher than for the case when only the sodium would be hydrogenated (∼1 mass% for x = 10). At 200 bar the onset of hydrogen absorption is observed at 150 °C. At a pressure of 1 bar hydrogen the major desorption starts at 250 °C and is completed at 300 °C (heating rate 1 °C min-1). This absorption and desorption temperatures are significantly reduced compared to pure C60, either due to a catalytic reaction of hydrogen on sodium or due to the negatively charged C60. The hydrogen ab/desorption is accompanied by a partial de/reintercalation of sodium. A minor part of the hydrogen is ionically bonded in NaH and the major part is covalently bonded in C60Hx. The sample can be fully dehydrogenated and no NaH is left after desorption. In contrast to C60, where the fullerene cages for high hydrogen loadings are destroyed during the sorption process, the NaxC60 sample stays intact. The samples were investigated by X-ray, in-situ neutron powder diffraction and infrared spectroscopy. NaxC60 was synthesized by reacting sodium azide (NaN3) with C60 (molar ratio of Na:C60 is 10:1). © 2012, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.

We report here on the preparation and characterization of a fullerenium salt in the solid state, where the fullerene is in the 2+ oxidized state. To succeed in this long-standing challenge, we exploit the oxidizing power of one of the strongest Lewis acids, AsF(5). The weak nucleophilic character of its conjugate base is essential in stabilizing the fullerene dication in a crystal lattice. High-resolution structural analysis of this compound, with the formula C(60)(AsF(6))(2), indicates that the highly reactive C(60)(2+) units are arranged according to a novel 1D "zigzag" polymer structure. The molecules are connected by an alternating sequence of four-membered carbon rings ([2 + 2] cycloaddition) and single C-C bonds. The long awaited high-T(c) superconductivity and magnetism, expected in a hole-doped C(60) compound, are replaced instead by a semiconducting behavior, quite probably originating from the reduced crystal and molecular symmetry upon polymerization. The small value of the energy gap (approximately 70 meV) suggests, nevertheless, the proximity of a metallic phase.

We report the extensive investigation of Li and H dynamics in Li6C60 and Li6C60Hy, by combining 7Li and 1H solid state NMR measurements with DC/AC conductivity, in order to evaluate the potential application of these systems for energy-storage purposes. 7Li NMR results show a local motion of Li ions above 200 K in both pristine and hydrogenated compounds, with activation energies of 90–150 meV and correlation times of about 30 ps. Evidences of Li interdiffusive dynamics are given by conductivity measurements in Li6C60 already above 120 K, with activation energies of 240 meV, suggesting that ionic conductivity is of the order of 10−5 S cm−1 at room temperature, with correlation times of about 150 ps. On the other hand, the Li6C60Hy behaves like a semiconductor with a high energy gap (ca. 2.5 eV), suggesting that diffusion of intercalated Li ions is prevented. 1H NMR measurements indicate the absence of H motions for the whole temperature range investigated (up to 360 K), neither on macroscopic or local scale. Li6C60 good properties for H2-storage are confirmed in terms of absorption capacity (5 wt% H2), moreover we found that around 35% of lithium segregates in LiH form, leaving Li4C60H40 as the final hydrogenation product.

Mixed ionic-electronic conductors (MIEC) are of growing interest for fuel cells, batteries and sensors. Here, by exploiting the unique properties of Li 4 C 60 2D fulleride and poly(ethylene oxide) (PEO), we demonstrate the feasibility of a MIEC where the nature of transport can be tuned from ionic, to mixed, to almost entirely electronic, simply by changing the weight ratio of the two basic components. By coupling 7 Li MAS-NMR, electrochemical impedance spectroscopy and open circuit voltage (OCV) measurements of a Li/composite/LiFePO 4 cell we demonstrate that: i) a fraction of Li + ions is extracted by Li 4 C 60 and confined into PEO amorphous strands similarly to what happens in PEO-salt systems; ii) a transition between prevalently ionic and electronic conductivity takes place at 33 wt% Li 4 C 60 . This new class of MIEC is very promising for the design of both chemically and electrochemically stable semi-cells and interfaces which can be employed in batteries and supercapacitors.

The possibility of producing magnetic graphene nanostructures by functionalization with aromatic radicals has been investigated. Functionalization of graphene basal plane was performed with three types of anilines: 4-bromoaniline, 4-nitroaniline and 4-chloroaniline. The samples were examined by composition analysis with energy-dispersive X-ray spectroscopy and magnetic measurements by SQUID magnetometry and electron paramagnetic resonance. Initial graphene was produced by thermal exfoliation. Both pristine and functionalized samples demonstrate strong paramagnetic contribution at low temperatures, which originates from intrinsic defects. Attachment of an organic molecule with the formation of a covalent bond with carbon atom on the basal plane generates a delocalized spin in the graphene pi - electron system. Nitroaniline proved to be the most suitable and sufficiently reactive to attach to the basal plane carbon atoms in large amounts. Functionalization of graphene with nitroaniline resulted in appearance both ferromagnetic and antiferromagnetic features with a clear antiferromagnetic transition near 120 K. (C) 2015 Elsevier B.V. All rights reserved.

Magnetic properties of graphene nanostructures functionalized with aromatic radicals were investigated by electron spin resonance (ESR) and superconducting quantum interference device (SQUID) techniques. Three types of functionalized graphene samples were investigated (functionalization was performed by 4-bromoaniline, 4-nitroaniline, or 4-chloroaniline). According to SQUID measurements, in case of functionalization by nitroaniline, sharp change in temperature dependence of magnetic susceptibility was observed near 120 K. Such behavior was explained as antiferromagnetic ordering. The same but more extended effect was observed in ESR measurements below 160 K. In the ESR measurements, only one resonance line with g-factor equal to 2.003 was observed. Based on the temperature dependencies of spin concentration and resonance position and intensity, the effect was explained as antiferromagnetic ordering along the extended defects on the basal planes of the graphene.

Using muon-spin spectroscopy, we study the exceptional dynamical properties of rotating molecular struts engineered within a Zn-based metal–organic framework at cryogenic temperatures, where the internal motions of almost any other organic substance are quenched. Muon-spin spectroscopy is particularly suited for this aim, as the experimental evidence suggests several implantation sites for the muons, among which at least one directly onto the rotating moiety. The dynamics of the molecular rotors are characterized by the exceptionally low activation energy EA ∼ 30 cal mol–1. At the same time, we evidence a highly unusual temperature dependence of the dipolar interaction of muons with nuclear magnetic moments on the rotors, suggesting a complex influence of the rotations on the muon implantation and diffusion.

Modification of graphene has been undertaken in many research contexts in order to improve its properties. In this study, we examine Ni-nanoparticles decoration on graphene and its effect on sodium-ion battery performance. A definite trend is observed on the relationship between Ni-nanoparticles concentration (and hence size) and battery performance. Comparable capacities on the order of 420 mAhg −1 after 20 cycles at 100 mAg −1 is observed for the 3 relatively high Ni-concentration samples NiC 10 , NiC 40 , and NiC 80 . As the Ni:C ratio decreases, a decreasing trend is observed in the measured capacity, with NiC 200 , NiC 500 , and NiC 1000 producing capacities of 350 mAhg −1 , 380 mAhg −1 , and 300 mAhg −1 respectively after 20 cycles at the same rate. Ex situ energy dispersive X-ray spectroscopy, scanning, and transmission electron microscopy shows the morphology of the Ni-nanoparticles decorated graphene and assists in quantifing their sodium content, emphasizing the increasing sodium content with increasing Ni-nanoparticles concentration. This systematic study details how Ni-nanoparticles concentration on graphene surfaces can be manipulated to enhance electrochemical performance, and that higher concentrations up to NiC 10 favour better performance. For a compromise between performance and cost (Ni cost), the best composition is NiC 500 which favors best performance with the least Ni decoration.

We herein report on the ability of fullerene C60 and hydrogenated fullerene C60Hx (x∼39) to operate as negative electrodes in novel Na-ion batteries. Building upon the known solubility of C60 in common organic electrolytes used in batteries, we developed a suitably optimized solid-state Na-(polyethylene oxide) electrolyte for this application. Electrochemical and structural properties of the fullerene electrodes were investigated through cyclic voltammetry, fixed-current charge/discharge of the electrodes, impedance spectroscopy and powder X-ray diffraction. Both C60 and hydrogenated C60 have been electrochemically intercalated with sodium. Specific capacities after the first cycle are 250 mAh g−1 and 230 mAh g−1 for C60 and C60Hx respectively. However, C60 electrode shows a strong irreversible character after the first discharge, probably due to the formation of stable polymeric NaxC60 phases, where Na+ ions diffusion is hindered. On the contrary, C60Hx displays better reversibility, suggesting that hydrogenation of the buckyball could be effective to preserve sufficiently large interstitial pathways for Na+ diffusion upon intercalation.