arXiv subjects

Vittorio Pellegrini

Publications and source records attributed to Vittorio Pellegrini.

At least 19 recordsLinked to original sources

arXiv2026

Graphene-based technologies for energy applications, challenges and perspectives

Here we report on technology developments implemented into the Graphene Flagship European project for the integration of graphene and graphene-related materials (GRMs) into energy application devices. Many of the technologies investigated so far aim at producing composite materials associating graphene or GRMs with either metal or semiconducting nanocrystals or other carbon nanostructures (e.g., CNT, graphite). These composites can be used favourably as hydrogen storage materials or solar cell absorbers. They can also provide better performing electrodes for fuel cells, batteries, or supercapacitors. For photovoltaic (PV) electrodes, where thin layers and interface engineering are required, surface technologies are preferred. We are using conventional vacuum processes to integrate graphene as well as radically new approaches based on laser irradiation strategies. For each application, the potential of implemented technologies is then presented on the basis of selected experimental and modelling results. It is shown in particular how some of these technologies can maximize the benefit taken from GRM integration. The technical challenges still to be addressed are highlighted and perspectives derived from the running works emphasized.

cond-mat.mtrl-sci↗

arXiv2025

The 2D Materials Roadmap

Over the past two decades, 2D materials have rapidly evolved into a diverse and expanding family of material platforms. Many members of this materials class have demonstrated their potential to deliver transformative impact on fundamental research and technological applications across different fields. In this roadmap, we provide an overview of the key aspects of 2D material research and development, spanning synthesis, properties and commercial applications. We specifically present roadmaps for high impact 2D materials, including graphene and its derivatives, transition metal dichalcogenides, MXenes as well as their heterostructures and moiré systems. The discussions are organized into thematic sections covering emerging research areas (e.g., twisted electronics, moiré nano-optoelectronics, polaritronics, quantum photonics, and neuromorphic computing), breakthrough applications in key technologies (e.g., 2D transistors, energy storage, electrocatalysis, filtration and separation, thermal management, flexible electronics, sensing, electromagnetic interference shielding, and composites) and other important topics (computational discovery of novel materials, commercialization and standardization). This roadmap focuses on the current research landscape, future challenges and scientific and technological advances required to address, with the intent to provide useful references for promoting the development of 2D materials.

cond-mat.mtrl-sci↗

arXiv2021

Graphene-Based Electrodes in a Vanadium Redox Flow Battery Produced by Rapid Low-Pressure Combined Gas Plasma Treatments

The development of high-power density vanadium redox flow batteries (VRFBs) with high energy efficiencies (EEs) is crucial for the widespread dissemination of this energy storage technology. In this work, we report the production of novel hierarchical carbonaceous nanomaterials for VRFB electrodes with high catalytic activity toward the vanadium redox reactions (VO2+/VO2+ and V2+/V3+). The electrode materials are produced through a rapid (minute timescale) low-pressure combined gas plasma treatment of graphite felts (GFs) in an inductively coupled radio frequency reactor. By systematically studying the effects of either pure gases (O2 and N2) or their combination at different gas plasma pressures, the electrodes are optimized to reduce their kinetic polarization for the VRFB redox reactions. To further enhance the catalytic surface area of the electrodes, single-/few-layer graphene, produced by highly scalable wet-jet milling exfoliation of graphite, is incorporated into the GFs through an infiltration method in the presence of a polymeric binder. Depending on the thickness of the proton-exchange membrane (Nafion 115 or Nafion XL), our optimized VRFB configurations can efficiently operate within a wide range of charge/discharge current densities, exhibiting energy efficiencies up to 93.9%, 90.8%, 88.3%, 85.6%, 77.6%, and 69.5% at 25, 50, 75, 100, 200, and 300 mA cm-2, respectively. Our technology is cost-competitive when compared to commercial ones (additional electrode costs < 100 euro m-2) and shows EEs rivalling the record-high values reported for efficient systems to date. Our work remarks on the importance to study modified plasma conditions or plasma methods alternative to those reported previously (e.g., atmospheric plasmas) to improve further the electrode performances of the current VRFB systems.

physics.app-ph↗

arXiv2021

Two-Dimensional Gallium Sulfide Nanoflakes for UV-Selective Photoelectrochemical-type Photodetectors

Two-dimensional (2D) transition-metal monochalcogenides have been recently predicted to be potential photo(electro)catalysts for water splitting and photoelectrochemical (PEC) reactions. Differently from the most established InSe, GaSe, GeSe, and many other monochalcogenides, bulk GaS has a large band gap of ca. 2.5 eV, which increases up to more than 3.0 eV with decreasing its thickness due to quantum confinement effects. Therefore, 2D GaS fills the void between 2D small-band-gap semiconductors and insulators, resulting of interest for the realization of van der Waals type-I heterojunctions in photocatalysis, as well as the development of UV light-emitting diodes, quantum wells, and other optoelectronic devices. Based on theoretical calculations of the electronic structure of GaS as a function of layer number reported in the literature, we experimentally demonstrate, for the first time, the PEC properties of liquid-phase exfoliated GaS nanoflakes. Our results indicate that solution-processed 2D GaS-based PEC-type photodetectors outperform the corresponding solid-state photodetectors. In fact, the 2D morphology of the GaS flakes intrinsically minimizes the distance between the photogenerated charges and the surface area at which the redox reactions occur, limiting electron-hole recombination losses. The latter are instead deleterious for standard solid-state configurations. Consequently, PEC-type 2D GaS photodetectors display a relevant UV-selective photoresponse. In particular, they attain responsivities of 1.8 mA W-1 in 1 M H2SO4 (at 0.8 V vs reversible hydrogen electrode -RHE-), 4.6 mA W-1 in 1 M Na2SO4 (at 0.9 V vs RHE), and 6.8 mA W-1 in 1 M KOH (at 1.1 V vs RHE) under 275 nm illumination wavelength with an intensity of 1.3 mW cm-2.

physics.app-ph↗

arXiv2021

Observation of flat bands in gated semiconductor artificial graphene

Flat bands near M points in the Brillouin zone are key features of honeycomb symmetry in artificial graphene (AG) where electrons may condense into novel correlated phases. Here we report the observation of van Hove singularity doublet of AG in GaAs quantum well transistors, which presents the evidence of flat bands in semiconductor AG. Two emerging peaks in photoluminescence spectra tuned by backgate voltages probe the singularity doublet of AG flat bands, and demonstrate their accessibility to the Fermi level. As the Fermi level crosses the doublet, the spectra display dramatic stability against electron density, indicating interplays between electron-electron interactions and honeycomb symmetry. Our results provide a new flexible platform to explore intriguing flat band physics.

cond-mat.mes-hall↗

arXiv2020

Scalable spray-coated graphene-based electrodes for high-power electrochemical double-layer capacitors operating over a wide range of temperature

Advancements in electrochemical double-layer capacitor (EDLC) technology require the concomitant use of novel efficient electrode materials and viable electrode manufacturing methods. Cost-effectiveness, scalability and sustainability are key-drivers for fulfilling product development chain accepted by worldwide legislations. Herein, we report a scalable and sprayable "green" electrode material-based ink based on activated carbon and single-/few-layer graphene (SLG/FLG) flakes. We show that, contrary to commercial reduced graphene oxide, defect-free and flat SLG/FLG flakes reduce the friction of ions over the electrode films, while spray coating deposition of our ink maximises the electrolyte accessibility to the electrode surface area. Sprayed SLG/FLG flakes-based EDLCs display superior rate capability performance (e.g., specific energies of 31.5, 23.7 and 12.5 Wh kg-1 at specific powers of 150, 7500 and 30000 W kg-1, respectively) compared to both SLG/FLG flakes-free devices and commercial-like EDLCs produced by slurry-coating method. The use of SLG/FLG flakes enables our sprayed EDLCs to operate in a wide range of temperature (-40/+100°C) compatible with ionic liquid/organic solvent-based electrolytes, overcoming the specific power limits of AC-based EDLCs. A prototype EDLCs stack consisting of multiple large-area EDLCs, each one displaying a capacitance of 25 F, demonstrates the industrial potential of our technology.

physics.app-ph↗

arXiv2020

Graphene Plasmonic Fractal Metamaterials for Broadband Photodetectors

Metamaterials have recently established a new paradigm for enhanced light absorption in state-of-the-art photodetectors. Here, we demonstrate broadband, highly efficient, polarization-insensitive, and gate-tunable photodetection at room temperature in a novel metadevice based on gold/graphene Sierpinski carpet plasmonic fractals. We observed an unprecedented internal quantum efficiency up to 100% from the near-infrared to the visible range with an upper bound of optical detectivity of $10^{11}$ Jones and a gain up to $10^{6}$, which is a fingerprint of multiple hot carriers photogenerated in graphene. Also, we show a 100-fold enhanced photodetection due to highly focused (up to a record factor of $|E/E_{0}|\approx20$ for graphene) electromagnetic fields induced by electrically tunable multimodal plasmons, spatially localized in self-similar fashion on the metasurface. Our findings give direct insight into the physical processes governing graphene plasmonic fractal metamaterials. The proposed structure represents a promising route for the realization of a broadband, compact, and active platform for future optoelectronic devices including multiband bio/chemical and light sensors.

physics.app-ph↗

arXiv2020

Solution-processed GaSe nanoflake-based films for photoelectrochemical water splitting and photoelectrochemical-type photodetectors

Gallium selenide (GaSe) is a layered compound, which has been exploited in nonlinear optical applications and photodetectors due to its anisotropic structure and pseudo-direct optical gap. Theoretical studies predicted that its two-dimensional (2D) form is a potential photocatalyst for water splitting reactions. Herein, we first report the photoelectrochemical (PEC) characterization of GaSe nanoflakes (single-/few-layer flakes), produced via liquid phase exfoliation, for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in both acidic and alkaline media. In 0.5 M H2SO4, the GaSe photoelectrodes display the best PEC performance, i.e. a ratiometric power-saved metric for HER (Φsaved,HER) of 0.09% and a ratiometric power-saved metric for OER (Φsaved,OER) of 0.25%. When used as PEC-type photodetectors, GaSe photoelectrodes show a responsivity of ~0.16 A W-1 upon 455 nm illumination at light intensity of 63.5 uW cm-2 and applied potential of -0.3 V vs. reversible hydrogen electrode (RHE). The stability analysis of the GaSe photodetectors evidences a durable operation over tens of cathodic linear sweep voltammetry scans in 0.5 M H2SO4 for HER. Viceversa, degradation effects have been observed in both alkaline and anodic operation due to highly oxidizing environment and O2-induced (photo-)oxidation effects. Our results provide new insight into PEC properties of GaSe nanoflakes for their exploitation in photoelectrocatalysis, PEC-type photodetectors and (bio)sensors.

physics.app-ph↗

arXiv2020

Flexible Graphene/Carbon Nanotube Electrochemical Double-Layer Capacitors with Ultrahigh Areal Performance

The fabrication of electrochemical double-layer capacitors (EDLCs) with high areal capacitance relies on the use of elevated mass loadings of highly porous active materials. Herein, we demonstrate a high-throughput manufacturing of graphene/nanotubes hybrid EDLCs. Wet-jet milling (WJM) method is exploited to exfoliate the graphite into single/few-layer graphene flakes (WJM-G) in industrial volume (production rate ~0.5 kg/day). Commercial single/double walled carbon nanotubes (SDWCNTs) are mixed with graphene flakes in order to act as spacers between the graphene flakes during their film formation. The latter is obtained by one-step vacuum filtration, resulting in self-standing, metal- and binder-free flexible EDLC electrodes with high active material mass loadings up to 30 mg cm-2. The corresponding symmetric WJM-G/SDWCNTs EDLCs exhibit electrode energy densities of 539 uWh cm-2 at 1.3 mW cm-2 and operating power densities up to 532 mW cm-2 (outperforming most of the EDLC technologies). The EDCLs show excellent cycling stability and outstanding flexibility even under highly folded states (up to 180 degrees). The combination of industrial-like production of active materials, simplified manufacturing of EDLC electrodes, and ultrahigh areal performance of the as-produced EDLCs are promising for novel advanced EDLC designs.

physics.app-ph↗

arXiv2020

Extending the colloidal transition metal dichalcogenide library to ReS2 nanosheets for application in gas sensing and electrocatalysis

Among the large family of transition metal dichalcogenides (TMDCs), recently ReS2 has stood out due to its nearly layer-independent optoelectronic and physicochemical properties. These are related to its 1T distorted octahedral structure, which leads to strong in-plane anisotropy and the presence of active sites at its surface, which makes ReS2 interesting for applications such as gas sensors and catalysts for H2 production. However, the current fabrication methods for ReS2 use chemical or physical vapor deposition (CVD or PVD) processes that are costly and involve complex and lengthy fabrication procedures, therefore limiting their large-scale production and exploitation. To address this issue, we developed a colloidal synthesis approach, which allows the production of ReS2 to be attained at temperatures below 360 Celsius degrees and with reaction times < 2 h, resulting in a more cost-efficient strategy than the CVD and PVD methods. By combining the solution-based synthesis with surface functionalization strategies, we demonstrate the feasibility of colloidal ReS2 nanosheet films for gas sensing of different toxic gases, moisture and other volatile compounds with highly competitive performance in comparison with devices built with CVD-grown ReS2 and MoS2. In addition, the integration of the ReS2 nanosheet films in assemblies, in which they are deposited on top of networks of carbon nanotubes, allowed us to fabricate electrodes for electrocatalysis for H2 production in both acid and alkaline conditions. Results from proof-of-principle devices show an electrocatalytic overpotential that is competitive with devices based on ReS2 produced by CVD, and even with MoS2, WS2 and MoSe2 electrocatalysts.

physics.app-ph↗

arXiv2020

Challenges and perspectives for new material solutions in batteries

We outline main challenges for future research in batteries, particularly, addressing the urgent needs of developing new environmentally friendly material solutions to enhance the energy density and safety of these storage devices. This will require embracing a multidisciplinary approach encompassing traditional electrochemistry and experimental solid-state physics, multiscale computational modelling, materials synthesis, and advanced characterization and testing

physics.app-ph↗

arXiv2020

Single-step exfoliation and functionalization of few-layers black phosphorus and its application for polymer composites

We demonstrate the large scale exfoliation of bulk black phosphorus into few-layers black phosphorus. We use wet-jet mill (WJM) as an industrially scalable exfoliation technique. In order to avoid the degradation by oxidation of the exfoliated flakes, the few-layers black phosphorus is protected by functionalisation (with 4-bromobenzene-diazonium tetrafluoroborate) during the exfoliation process. We used the exfoliated and functionalised flakes as fillers in a polymethyl methacrylate matrix to test the mechanical endurance, obtaining an improvement in the Young modulus of 106% compared to the bare polymer. These data support the development of black phosphorus materials as 2D-polymer fillers and performance-enhancers.

physics.app-ph↗

arXiv2019

CVD-graphene/graphene flakes dual-films as advanced DSSC counter electrodes

The use of graphene-based electrodes is burgeoning in a wide range of applications, including solar cells, light emitting diodes, touch screens, field-effect transistors, photodetectors, sensors and energy storage systems. The success of such electrodes strongly depends on the implementation of effective production and processing methods for graphene. In this work, we take advantage of two different graphene production methods to design an advanced, conductive oxide- and platinum-free, graphene-based counter electrode for dye-sensitized solar cells (DSSCs). In particular, we exploit the combination of a graphene film, produced by chemical vapor deposition (CVD) (CVD-graphene), with few-layer graphene (FLG) flakes, produced by liquid phase exfoliation. The CVD-graphene is used as charge collector, while the FLG flakes, deposited atop by spray coating, act as catalyst for the reduction of the electrolyte redox couple (i.e., I3-/I-- and Co+2/+3). The as-produced counter electrodes are tested in both I3-/I-- and Co+2/+3-based semitransparent DSSCs, showing power conversion efficiencies of 2.1% and 5.09%, respectively, under 1 SUN illumination. At 0.1 SUN, Co+2/+3-based DSSCs achieve a power conversion efficiency as high as 6.87%. Our results demonstrate that the electrical, optical, chemical and catalytic properties of graphene-based dual films, designed by combining CVD-graphene and FLG flakes, are effective alternatives to FTO/Pt counter electrodes for DSSCs for both outdoor and indoor applications.

physics.app-ph↗

arXiv2019

Liquid-phase exfoliated indium-selenide flakes and their application in hydrogen evolution reaction

Single- and few-layered InSe flakes are produced by the liquid-phase exfoliation of beta-InSe single crystals in 2-propanol, obtaining stable dispersions with a concentration as high as 0.11 g/L. Ultracentrifugation is used to tune the morphology, i.e., the lateral size and thickness of the as-produced InSe flakes. We demonstrate that the obtained InSe flakes have maximum lateral sizes ranging from 30 nm to a few um, and thicknesses ranging from 1 to 20 nm, with a max population centred at ~ 5 nm, corresponding to 4 Se-In-In-Se quaternary layers. We also show that no formation of further InSe-based compounds (such as In2Se3) or oxides occurs during the exfoliation process. The potential of these exfoliated-InSe few-layer flakes as a catalyst for hydrogen evolution reaction (HER) is tested in hybrid single-walled carbon nanotubes/InSe heterostructures. We highlight the dependence of the InSe flakes morphologies, i.e., surface area and thickness, on the HER performances achieving best efficiencies with small flakes offering predominant edge effects. Our theoretical model unveils the origin of the catalytic efficiency of InSe flakes, and correlates the catalytic activity to the Se vacancies at the edge of the flakes.

cond-mat.mtrl-sci↗

arXiv2019

WS2-graphite dual-ion battery

A novel WS2-graphite dual-ion battery (DIB) is developed by combining together a conventional graphite cathode and high-capacity few-layer WS2 flakes anode. The WS2 flakes are produced by exploiting wet-jet milling (WJM) exfoliation, which allows mass production of few-layer WS2 flakes in dispersion, with an exfoliation yield of 100%. The WS2-anodes enable DIBs, based on hexafluorophosphate (PF6-) and lithium (Li+) ions, to achieve charge specific capacities of 457, 438, 421, 403, 295 and 169 mAh g-1 at current rates of 0.1, 0.2, 0.3, 0.4, 0.8 and 1.0 A g-1, respectively, outperforming conventional DIBs. The WS2-based DIBs operate in the 0 to 4 V cell voltage range, thus extending the operating voltage window of conventional WS2-based Li-ion batteries (LIBs). These results demonstrate a new route towards the exploitation of WS2, and possibly other transition metal dichalcogenides (TMDs), for the development of next-generation energy storage devices.

cond-mat.mtrl-sci↗

arXiv2019

Quantum supercapacitors

Recently there has been a great deal of interest on the possibility to exploit quantum-mechanical effects to increase the performance of energy storage systems. Here we introduce and solve a model of a quantum supercapacitor. This consists of two chains, one containing electrons and the other one holes, hosted by arrays of double quantum dots, the latter being a building block of experimental architectures for realizing charge and spin qubits. The two chains are in close proximity and embedded in the same photonic cavity, which is responsible for long-range coupling between all the qubits, in the same spirit of the Dicke model. By employing a variational approach, we find the phase diagram of the model, which displays ferromagnetic and antiferromagnetic phases for suitable pseudospin degrees of freedom, together with phases characterized by collective superradiant behavior. Importantly, we show that when transitioning from the ferro/antiferromagnetic to the superradiant phase, the quantum capacitance of the model is greatly enhanced. Our work offers opportunities for the experimental realization of a novel class of quantum supercapacitors with an enhanced storing power stemming from exquisite quantum mechanical effects.

cond-mat.mes-hall↗

arXiv2018

Charger-mediated energy transfer in exactly-solvable models for quantum batteries

We present a systematic analysis and classification of several models of quantum batteries involving different combinations of two level systems and quantum harmonic oscillators. In particular, we study energy transfer processes from a given quantum system, termed charger, to another one, i.e. the proper battery. In this setting, we analyze different figures of merit, including the charging time, the maximum energy transfer, and the average charging power. The role of coupling Hamiltonians which do not preserve the number of local excitations in the charger-battery system is clarified by properly accounting them in the global energy balance of the model.

quant-ph↗

arXiv2018

Towards 'Pt-free' Anion-Exchange Membrane Fuel Cells: Fe-Sn Carbon Nitride-Graphene 'Core-Shell' Electrocatalysts for the Oxygen Reduction Reaction

We report on the development of two new Pt-free electrocatalysts (ECs) for the oxygen reduction reaction (ORR) based on graphene nanoplatelets (GNPs). We designed the ECs with a core-shell morphology, where a GNP core support is covered by a carbon nitride (CN) shell. The proposed ECs present ORR active sites that are not associated to nanoparticles of metal/alloy/oxide, but are instead based on Fe and Sn sub-nanometric clusters bound in coordination nests formed by carbon and nitrogen ligands of the CN shell. The performance and reaction mechanism of the ECs in the ORR are evaluated in an alkaline medium by cyclic voltammetry with the thin-film rotating ring-disk approach and confirmed by measurements on gas-diffusion electrodes. The proposed GNP-supported ECs present an ORR overpotential of only ca. 70 mV higher with respect to a conventional Pt/C reference EC including a XC-72R carbon black support. These results make the reported ECs very promising for application in anion-exchange membrane fuel cells. Moreover, our methodology provides an example of a general synthesis protocol for the development of new Pt-free ECs for the ORR having ample room for further performance improvement beyond the state of the art.

physics.chem-ph↗