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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

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Journal of Energy Chemistry 2020年第10期29卷 22-32页

作者： Shiming Chen Siglinda Perathoner Claudio Ampelli Hua Wei salvatore abate Bingsen Zhang Gabriele Centi Dept.ChimBioFarAM 98166 MessinaItaly Dalian Institute of Chemical Physics Chinese Academy of SciencesDalian 116023LiaoningChina Catalysis and Materials Division Institute of Metal ResearchChinese Academy of Sciences(IMR CAS)Shenyang Dept.MIFT(Industrial University of Messina ERIC aisbl and INSTM/CASPE98166 MessinaItaly

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 *** 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 *** 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 *** electrocatalyst was stable at least 12 h at the working *** by switching N2 to Ar evidence that ammonia was formed from the gas-phase *** 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 *** 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 *** 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.

关键词： Ammonia direct synthesis Electrochemical activation Heterogeneous catalysis Active sites N2 electrocatalytic conversion

Electrocatalytic production of glycolic acid via oxalic acid reduction on titania debris supported on a TiO_(2)nanotube array

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Journal of Energy Chemistry 2022年第5期31卷 669-678页

作者： Francesco Pio Abramo Federica De Luca Rosalba Passalacqua Gabriele Centi Gianfranco Giorgianni Siglinda Perathoner salvatore abate Department of ChiBioFarAM(Industrial Chemistry) University of MessinaERIC aisbl and INSTM/CASPEV.le F.Stagno d’Alcontres 31Messina 98166Italy University of Calabria Department of Environmental EngineeringLaboratory of Industrial Chemistry and Catalysis Via P.Bucci87036 RendeCSItaly

Electrodes prepared by anodic oxidation of Ti foils are robust and not toxic materials for the electrocatalytic reduction of oxalic acid to glycolic acid, allowing the development of a renewable energy-driven process for producing an alcoholic compound from an organic acid at low potential and room temperature. Coupled with the electrochemical synthesis of the oxalic acid from CO_(2),this process represents a new green and low-carbon path to produce added value chemicals from CO_(2). Various electrodes prepared by anodic oxidation of Ti foils were investigated. They were characterized by the presence of a TiO_(2) nanotube array together with the presence of small patches, debris, or TiO_(2) nanoparticles. The concentration of oxygen vacancies, the amount of Ti^(3+) measured by X-ray photoelectron spectroscopy(XPS) and the intensity of the anodic peak measured by cyclic voltammetry, were positively correlated with the achieved oxalic acid conversion and glycolic acid yield. The analysis of the results indicates the presence of small amorphous TiO_(2) nanoparticles(or surface patches or debris) interacting with TiO_(2) nanotubes, the sites responsible for the conversion of oxalic acid and glycolic acid yield. By varying this structural characteristic of the electrodes, it is possible to tune the glycolic acid to glyoxylic acid relative ratio. A best cumulative Faradaic efficiency(FE) of about 84% with FE to glycolic acid around 60% and oxalic conversion about 30% was observed.

关键词： Oxalic acid TiO_(2)nanotubes Glyoxylic acid Glycolic acid Electrocatalysis

The energy-chemistry nexus: A vision of the future from sustainability perspective

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Journal of Energy Chemistry 2015年第5期24卷 535-547页

作者： salvatore abate Gabriele Centi Paola Lanzafame Siglinda Perathoner Department of DIECII Section Industrial Chemistry University of Messina INSTM/CASPE (Laboratory of Catalysis for Sustainable Production and Energy) and ERIC aisbl (European Research Institute of Catalysis)

The changing energy-chemistry nexus is discussed in this perspective paper about the future of sustainable energy and chemical production to identify the priorities and open issues on which focus research and development. Topics discussed regard （i） the new sustainable energy scenario, （ii） the role of energy storage （from smart grids to chemical storage of energy）, （iii） the outlooks and role of solar （bio）refineries and solar fuels, （iv） how to integrate hio- and solar-refineries to move to new economy, （v） the role of methanol at the crossover of new energy-chemistry nexus, （vi） the role of chemistry in this new scenario, （vii） the role of nanomaterials for a sustainable energy, （viii） the use of nanocarbons to design advanced energy conversion and storage devices, and （ix） possibilities and routes to exploit solar energy and methane （shale gas）. The contribution provides a glimpse of the emerging directions and routes with some elements about their possible role in the future scenario, but does not orovide a detailed analysis of the state of the art in these directions

关键词： Energy Chemistry Future scenario Catalysis Sustainability

Role of size and pretreatment of Pd particles on their behaviour in the direct synthesis of H_2O_2

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Journal of Energy Chemistry 2016年第2期25卷 295-303页

作者： salvatore abate Katia Barbera Gabriele Centi Gianfranco Giorgianni Siglinda Perathoner University of Messina ERIC aisbl and INSTMCASPE Section Industrial Chemistry

Two families of catalysts, based on Pd nanoparticles supported on ceramic asymmetric tubular alumina membranes, are studies in the direct synthesis of H2O2. They are prepared by depositing Pd in two ways：（i） reduction with N2H4 in an ultrasonic bath and（ii） by impregnation-deposition. The first preparation leads to larger particles, with average size of around 11 nm, while the second preparation leads to smaller particles, with average size around 4 nm. The catalytic membranes were tested as prepared, after thermal treatment in air and after further pre-reduction with H2 in mild（100 ℃） conditions. Samples were characterized by TEM, CO-chemisorption monitored by DRIFTS method and TPR, while catalytic tests have been performed in a semi-batch recirculation membrane reactor. Experimental catalytic results were analysed using two kinetics models to derive the reaction constants for the parallel and consecutive reactions of the kinetic network. Smaller particles of Pd show lower selectivity due to the higher rate of parallel combustion, even if the better dispersion of Pd and thus higher metal surface area in the sample lead to a productivity in H2O2 similar or even higher than the sample with the larger Pd particles. Independently on the presence of smaller or larger Pd nanoparticles, an oxidation treatment leads to a significant enhancement in the productivity, although the catalyst progressively reduces during the catalytic process. The inhibition of the parallel combustion reaction（to water） induced from the calcination treatment remains after the in-situ reduction of the oxidized Pd species formed during the *** is likely due to the elimination of defect sites which dissociatively activate oxygen, and tentatively attributed to Pd sites able to give three- and four-fold coordination of CO.

关键词： H2O2 direct synthesis Pd nanoparticles Kinetics of H2O2 synthesis Pd role in H2O2 synthesis

Misfolded amyloid-beta conformational variants(strains)as drivers of Alzheimer's disease neuropathology

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Neural Regeneration Research 2025年第11期20卷 3219-3220页

作者： salvatore Saieva Rodrigo Morales Department of Neurology The University of Texas Health Science Center at HoustonHoustonTXUSA Centro Integrativo de Biologia y Quimica Aplicada(CIBQA) Universidad Bernardo O’HigginsSantiagoChile

Pathological and clinical variability in Alzheimer's disease(AD):AD is clinically cha racterized by progressive memory loss and cognitive *** a pathological point of view,the main features of AD are the deposition of amyloid plaques(composed of amyloid-beta,Aβ)and neurofibrillary tangles containing hyperphosphorylated Tau in the brain,accompanied by neu ronal and synaptic loss,neuroinflammation and brain atrophy(Jellinger,2022).Regardless of these common traits,growing evidence shows increased heterogen eity in the brain of AD patients considering both clinical manifestations and pathological features.

关键词： amyloid Alzheimer clinical

Virtual internal thermal work evaluation in the multifield variational statements for the analysis of multilayered structures

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Journal of Zhejiang University-Science A(Applied Physics & Engineering) 2013年第5期14卷 317-326页

作者： salvatore BRISCHETTO Department of Mechanical and Aerospace Engineering Politecnico di TorinoCorso Duca degli Abruzzi 2410129 TorinoItaly

The principle of virtual displacements(PVDs)extended to elasto-thermo-electric problems includes virtual internal elastic,thermal and electric *** governing equations have displacement vector,temperature and electric potential as primary variables of the problem,and the elasto-thermal,elasto-electric and pure elastic problems are obtained as particular cases by deleting the appropriate contributions in the general elasto-thermo-electric variational *** most sensitive issue is given by thermal coupling because the thermo-elastic and thermo-electric effects change depending on the type of load and analysis considered(mechanical load,temperature or electric potential imposed and free vibration analysis).This feature means that the form of the virtual internal thermal work in such variational statements changes depending on the analysis performed and the load *** about multilayered plates and shells suggest the appropriate extension of the variational statement for each analysis,and they give an exhaustive explanation for several forms of the PVD proposed.

关键词： Principle of virtual displacements(PVDs) Variational statements Elasto-thermo-electric problems Multilayered structures Virtual internal elastic work Virtual internal thermal work Virtual internal electric work

A Continuum Shell Model Including van derWaals Interaction for Free Vibrations of Double-Walled Carbon Nanotubes

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Computer Modeling in Engineering & Sciences 2015年第4期104卷 305-327页

作者： salvatore Brischetto Department of Mechanical and Aerospace Engineering Politecnico di TorinoCorso Duca degli Abruzzi2410129 TorinoITALY

This paper proposes the free vibration analysis of Double-Walled Carbon NanoTubes(DWCNTs).A continuum elastic three-dimensional shell model is used for natural frequency investigation of simply supported *** 3D shell method is compared with beam analyses to show the applicability limits of 1D beam *** effect of van der Waals interaction between the two cylinders is shown for different Carbon NanoTube(CNT)lengths and vibration *** give the van der Waals interaction effect in terms of frequency *** order to apply the 3D shell continuum model,DWCNTs are defined as two concentric isotropic cylinders(with an equivalent thickness and Young modulus)which can be linked by means of the interlaminar continuity conditions or by means of an infinitesimal fictitious layer which represents the van der Waals interaction.

关键词： Exact solution three-dimensional shell model double-walled carbon nanotube van der Waals interaction free vibration

Further studies on “magnetosensitive bacteria”

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Chinese Journal of Oceanology and Limnology 2009年第1期27卷 6-12页

作者： salvatore BELLINI Institute of Microbiology University of Pavia

Various experimental techniques for study of magnetosensitive bacteria are described and the experimental results are presented and discussed.

关键词： magnetosensitive bacteria biomagnetic microerophilic oxygen

SUSY QM in a One-Dimensional Box and Local Observable Quantities

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Chinese Physics Letters 2006年第8期23卷 1969-1972页

作者： salvatore De Vincenzo Escuela de Fisica Facultad de Ciencias Universidad Central de Venezuela A.P. 47145 Caracas 1041-A Venezuela

We investigate several Hamiltonians for a free particle in a one-dimensional box, in the context of supersymmetric quantum mechanics. Specifically, we study this problem with the Neumann boundary condition, the periodic and antiperiodic boundary condition, and some mixed and complex boundary conditions. This is achieved by using an approach recently proposed which expresses the factorization of the partner Hamiltonians in terms of the probability density and current for the ground-state eigenfunction of one of them.

关键词： SUPERSYMMETRIC QUANTUM-MECHANICS BOUNDARY-CONDITIONS ENERGY-SPECTRA SUPERPOTENTIALS FACTORIZATION POTENTIALS PARTICLE SYSTEMS