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| 1 | Electrocatalytic conversion of CO_2 to liquid fuels using nanocarbon-based electrodes显示文摘Recent advances on the use of nanocarbon-based electrodes for the electrocatalytic conversion of gaseous streams of CO2 to liquid fuels are discussed in this perspective paper. A novel gas-phase electrocatalytic cell, different from the typical electrochemical systems working in liquid phase, was developed. There are several advantages to work in gas phase, e.g. no need to recover the products from a liquid phase and no problems of CO2 solubility, etc. Operating under these conditions and using electrodes based on metal nanoparticles supported over carbon nanotube (CNT) type materials, long C-chain products (in particular isopropanol under optimized conditions, but also hydrocarbons up to C8-C9) were obtained from the reduction of CO2 . Pt-CNT are more stable and give in some cases a higher productivity, but Fe-CNT, particular using N-doped carbon nanotubes, give excellent properties and are preferable to noble-metal-based electrocatalysts for the lower cost. The control of the localization of metal particles at the inner or outer surface of CNT is an importact factor for the product distribution. The nature of the nanocarbon substrate also plays a relevant role in enhancing the productivity and tuning the selectivity towards long C-chain products. The electrodes for the electrocatalytic conversion of CO2 are part of a photoelectrocatalytic (PEC) solar cell concept, aimed to develop knowledge for the new generation artificial leaf-type solar cells which can use sunlight and water to convert CO2 to fuels and chemicals. The CO2 reduction to liquid fuels by solar energy is a good attempt to introduce renewables into the existing energy and chemical infrastructures, having a higher energy density and easier transport/storage than other competing solutions (i.e. H2 ). | Chiara Genovese Claudio Ampelli Siglinda Perathoner Gabriele Centi | 2013 | Journal of Energy Chemistry2013，22，2： | 4 |
| 2 | 碳基催化剂:为开发下一代纳米工程催化材料开辟新方法(英文)显示文摘This essay analyses some of the recent development in nanocarbons (carbon materials having a defined and controlled nano-scale dimension and functional properties which strongly depend on their nano-scale features and architecture), with reference to their use as advanced catalytic materials. It is remarked how their features open new possibilities for catalysis and that they represent a new class of catalytic materials. Although carbon is used from long time in catalysis as support and electrocatalytic applications, nanocarbons offer unconventional ways for their utilization and to address some of the new challenges deriving from moving to a more sustainable future. This essay comments how nanocarbons are a key element to develop next-generation catalytic materials, but remarking that this goal requires overcoming some of the actual limits in current research. Some aspects are discussed to give a glimpse on new directions and needs for R&D to progress in this direction. | Claudio Ampelli Siglinda Perathoner Gabriele Centi | 2014 | 催化学报2014，35，6： | 3 |
| 3 | Enhanced performance in the direct electrocatalytic synthesis of ammonia from N2 and H2O by an in-situ electrochemical activation of CNT-supported iron oxide nanoparticles显示文摘The direct electrocatalytic synthesis of ammonia from N2 and H2O by using renewable energy sources and ambient pressure/temperature operations is a breakthrough technology,which can reduce by over 90%the greenhouse gas emissions of this chemical and energy storage process.We report here an in-situ electrochemical activation method to prepare Fe2O3-CNT(iron oxide on carbon nanotubes)electrocatalysts for the direct ammonia synthesis from N2 and H2O.The in-situ electrochemical activation leads to a large increase of the ammonia formation rate and Faradaic efficiency which reach the surprising high values of 41.6μg mgcat^−1 h^−1 and 17%,respectively,for an in-situ activation of 3 h,among the highest values reported so far for non-precious metal catalysts that use a continuous-flow polymer-electrolytemembrane cell and gas-phase operations for the ammonia synthesis hemicell.The electrocatalyst was stable at least 12 h at the working conditions.Tests by switching N2 to Ar evidence that ammonia was formed from the gas-phase nitrogen.The analysis of the changes of reactivity and of the electrocatalyst characteristics as a function of the time of activation indicates a linear relationship between the ammonia formation rate and a specific XPS(X-ray-photoelectron spectroscopy)oxygen signal related to O2−in iron-oxide species.This results together with characterization data by TEM and XRD suggest that the iron species active in the direct and selective synthesis of ammonia is a maghemite-type iron oxide,and this transformation from the initial hematite is responsible for the in-situ enhancement of 3-4 times of the TOF(turnover frequency)and NH3 Faradaic efficiency.This transformation is likely related to the stabilization of the maghemite species at CNT defect sites,although for longer times of preactivation a sintering occurs with a loss of performances. | Shiming Chen Siglinda Perathoner Claudio Ampelli Hua Wei Salvatore Abate Bingsen Zhang Gabriele Centi | 2020 | Journal of Energy Chemistry2020，29，10： | 2 |
| 4 | Calorimetric study of the inhibition of runaway reactions during methylmethacrylate polymerization processes显示文摘 | Claudio Ampelli Dehorn Di Bella Giuseppe Maschlo | 2006 | Journal of Loss Prevention in the Process Industries2006，19，5： | 1 |
| 5 | Photoactive materials based on semiconducting nanocarbons——A challenge opening new possibilities for photocatalysis显示文摘This perspective paper introduces the concept that nanocarbons and related materials such as carbon dots are an interesting intrinsic photocatalytic semiconducting material, and not only a modifier of the existing(semiconducting) materials to prepare hybrid materials. The semiconducting properties of the nanocarbons, and the possibility to have the band gap within the visible-light region through defect band engineering, introduction of light heteroatoms and control/manipulation of the curvature or surface functionalization are discussed. These materials are conceptually different from the 'classical' semiconducting photocatalysts, because semiconductor domains with tuneable characteristics are embedded in a conductive carbon matrix, with the presence of various functional groups(as C=O groups) enhancing charge separation by trapping electrons. These nanocarbons open a range of new possibilities for photocatalysis both for energetic and environmental applications. The use of nanocarbons as quantum dots and photoluminescent materials was also analysed. | Siglinda Perathoner Claudio Ampelli Shiming Chen Rosalba Passalacqua Dangsheng Su Gabriele Centi | 2017 | Journal of Energy Chemistry2017，26，2： | 0 |
| 6 | Analysis of the factors controlling performances of Au-modified TiO2 nanotube array based photoanode in photo-electrocatalytic(PECa)cells显示文摘The efficiency of photo-electrocatalytic(PECa) devices for the production of solar fuels depends on several limiting factors such as light harvesting, charge recombination and mass transport diffusion. We analyse here how they influence the performances in PECa cells having a photo-anode based on Au-modified TiO_2 nanotube(TNT) arrays, with the aim of developing design criteria to optimize the photo-anode and the PECa cell configuration for water photo-electrolysis(splitting) and ethanol photo-reforming processes.The TNT samples were prepared by controlled anodic oxidation of Ti foils and then decorated with gold nanoparticles using different techniques to enhance the visible light response through heterojunction and plasmonic effects. The activity tests were made in a gas-phase reactor, as well as in a PECa cell without applied bias. Results were analysed in terms of photo-generated current, H_2 production rate and photoconversion efficiency. Particularly, a solar-to-hydrogen efficiency of 0.83% and a Faradaic efficiency of 91%were obtained without adding sacrificial reagents. | Claudio Ampelli Francesco Tavella Chiara Genovese Siglinda Perathoner Marco Favaro Gabriele Centi | 2017 | Journal of Energy Chemistry2017，26，2： | 0 |
| 7 | CO_(2)conversion to solar fuels and chemicals:Opening the new paths显示文摘This future article discusses the new prospects and directions of CO_(2)conversion via the photo-electrocatalytic(PEC)route.The second(2nd)generation solar fuels and chemicals(SFs)are generated directly in PEC systems via electrons/protons reactions without forming molecular H_(2)as an intermediate,overcoming the thermodynamics limitations and practical issues encountered for electro-fuels produced by multistep thermocatalytic processes(i.e.CO_(2)conversion with H_(2)coming from water electrolysis).A distributed and decentralized production of SFs requires very compact,highly integrated,and intensified technologies.Among the existing reactors of advanced design(based on artificial leaves or photosynthesis),the integrated photovoltaic plus electrocatalytic(PV-EC)device is the only system(demonstrated at large scale)to produce SFs with high solar-to-fuel(STF)efficiency.However,while the literature indicates STF efficiency as the main(and only)measure of process performance,we remark here the need to refer to productivity(in terms of current density)and make tests with reliable flow PEC systems(with electrodes of at least 5–10 cm^(2))to accelerate the scaling-up process.Using approaches that minimize downstream separation costs is also mandatory.Many limitations exist in PEC systems,but most can be overcome by proper electrode and cell engineering,thus going beyond the properties of the electrocatalysts.As examples of current developments,we present the progress of(i)artificial leaf/tree devices for green H_(2)distributed production and(ii)a PEC device producing the same chemicals at both cathode and anode parts without downstream operations for green solvent distributed production.Based on these developments,future directions,such as producing fertilizers and food components from the air,are outlined.The aim is to provide new ideas and research directions from a personal perspective. | Gabriele Centi Claudio Ampelli | 2024 | Journal of Energy Chemistry2024，91，4： | 0 |
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