72 research outputs found
Electrochemical properties of oxygen-enriched carbon-based nanomaterials
The introduction of oxygen moieties on a carbon-based material to enhance the electrode material activity for the oxygen reduction reaction (ORR) is a most unexplored experimental approach due to the risk of reducing the electron-transport ability of the electrode material. Herein, it is shown that carbon nanomaterials generated electrochemically from graphite can simultaneously show an anomalous high content of oxygen functionalities and a high heterogeneous electron transfer rate. This study was demonstrated with a set of four samples, prepared at different galvanostatic conditions. All the samples display a non-ordered carbon network dominated by aromatic rings, an O/C ratio greater than 0.4, but different amounts of various oxygen-containing functionalities. The electron-transport properties of the obtained films were appraised by cyclic voltammetry and electrochemical impedance spectroscopy.
The application of these metal-free electrode materials to the ORR in the alkaline medium has shown a direct correlation between the materials catalytic activity (potential onset, kinetic current and number of electrons transferred) and the Cdouble bondO amount, whereas a negative correlation was found for Csingle bondO. Their excellent ability for the H2O2 reduction was also demonstrated. This work opens a new perspective on the use of highly oxidized carbon nanomaterials in electrocatalysis.publishe
TiO 2
Nanocomposites TiO2-CdS with different relative contents of CdS (molar ratios Cd/Ti = 0.02, 0.03, 0.05, 0.1, 0.2, and 0.5) were studied. The structural, photophysical, and chemical properties were investigated using XRD, Raman spectroscopy, XPS, GSDR, and LIL. XRD and Raman results confirmed the presence of TiO2 and CdS with intensities dependent on the ratio Cd/Ti. The presence of CdSO4 was detected by XPS at the surface of all TiO2-CdS composites. The relative amount of sulphate was dependent on the CdS loading. Luminescence time-resolved spectra clearly proved the existence of an excitation transfer process from CdS to TiO2 through the luminescence emission from TiO2 after excitation of CdS at λexc=410 nm, where no direct excitation of TiO2 occurs. Photodegradation of a series of aromatic carboxylic acids—benzoic, salicylic, 4-bromobenzoic, 3-phenylpropionic, and veratric acids—showed a great enhancement in the photocatalytic efficiency of the TiO2-CdS composites, which is due, mainly, to the effect of the charge carriers’ increased lifetime. In addition, it was shown that the oxidation of CdS to CdSO4 did not result in the deactivation of the photocatalytic properties and even contributed to enhance the degradation efficiency
A Comparative Study
This research was funded by EU funds through the FEDER European Regional Development Fund (project LISBOA-02-0145-FEDER-031311) project LA/P/0056/2020 of Institute of Molecular Sciences, and LA/P/0140/2020 of i4HB, project UID/EEA/00066/2020 from the Center of Technology and Systems, and from the Instituto Politécnico de Lisboa with IPL/2018/STREAM_ISEL and IPL/2020/AGE-SPReS_ISEL projects. APCR and AMF thank the Instituto Superior Técnico for the scientific employment contracts IST-ID/119/2018 and IST-ID/131/2018, respectively.
Publisher Copyright:
© 2022 by the authors. Licensee MDPI, Basel, Switzerland.Aiming to develop a nanoparticle-based optical biosensor using gold nanoparticles (AuNPs) synthesized using green methods and supported by carbon-based nanomaterials, we studied the role of carbon derivatives in promoting AuNPs localized surface plasmon resonance (LSPR), as well as their morphology, dispersion, and stability. Carbon derivatives are expected to work as immobi-lization platforms for AuNPs, improving their analytical performance. Gold nanoparticles (AuNPs) were prepared using an eco-friendly approach in a single step by reduction of HAuCl4·3H2O using phytochemicals (from tea) which act as both reducing and capping agents. UV–Vis spectroscopy, transmission electron microscopy (TEM), zeta potential (ζ-potential), and X-ray photoelectron spectroscopy (XPS) were used to characterize the AuNPs and nanocomposites. The addition of reduced graphene oxide (rGO) resulted in greater dispersion of AuNPs on the rGO surface compared with carbon-based nanomaterials used as a support. Differences in morphology due to the nature of the carbon support were observed and are discussed here. AuNPs/rGO seem to be the most promising candidates for the development of LSPR biosensors among the three composites we studied (AuNPs/G, AuNPs/GO, and AuNPs/rGO). Simulations based on the Mie scattering theory have been used to outline the effect of the phytochemicals on LSPR, showing that when the presence of the residuals is limited to the formation of a thin capping layer, the quality of the plasmonic resonance is not affected. A further discussion of the application framework is presented.publishersversionpublishe
Prospects for microwave plasma synthesized N-graphene in secondary electron emission mitigation applications
PTDC/NAN-MAT/30565/2017
D01-284/2019 (INFRAMAT)
IBB BASE 2020-2023
UID/FIS/00068/2019.The ability to change the secondary electron emission properties of nitrogen-doped graphene (N-graphene) has been demonstrated. To this end, a novel microwave plasma-enabled scalable route for continuous and controllable fabrication of free-standing N-graphene sheets was developed. High-quality N-graphene with prescribed structural qualities was produced at a rate of 0.5 mg/min by tailoring the high energy density plasma environment. Up to 8% of nitrogen doping levels were achieved while keeping the oxygen content at residual amounts ( 1%). The synthesis is accomplished via a single step, at atmospheric conditions, using ethanol/methane and ammonia/methylamine as carbon and nitrogen precursors. The type and level of doping is affected by the position where the N-precursor is injected in the plasma environment and by the type of precursors used. Importantly, N atoms incorporated predominantly in pyridinic/pyrrolic functional groups alter the performance of the collective electronic oscillations, i.e. plasmons, of graphene. For the first time it has been demonstrated that the synergistic effect between the electronic structure changes and the reduction of graphene $-plasmons caused by N doping, along with the peculiar “crumpled” morphology, leads to sub-unitary (textless 1) secondary electron yields. N-graphene can be considered as a prospective low secondary electron emission and plasmonic material.publishersversionpublishe
Novel organotin-PTA complexes supported on mesoporous carbon materials as recyclable catalysts for solvent-free cyanosilylation of aldehydes
The work was also funded by national funds through FCT, under the Scientific Employment Stimulus-Institutional Call (CEEC-INST/00102/2018).
AGM is grateful to Associação do Instituto Superior Técnico para a Investigação e Desenvolvimento ( IST-ID ) for his post-doctoral fellowship through grant no. BL133/2021-IST-ID . AP and AMF are grateful to FCT and Instituto Superior Técnico (IST), Portugal through DL/57/2017 (Contract no. IST-ID/197/2019 and IST-ID/131/2018). This publication is also supported by the RUDN University Strategic Academic Leadership Program (recipient AJLP, preparation). The authors also acknowledge the Portuguese NMR Network (IST-UL Centre) for access to the NMR facility.
Publisher Copyright:
© 2023 Elsevier B.V.New organotin compounds with general formula [(PTA-CH2-C6H4-p-COO)SnR3]Br (where R is Me for 3 and Ph for 4; PTA = 1,3,5-triaza-7-phosphaadamantane), bearing the methylene benzoate PTA derivative, were synthesized through a mild two-step process. The compounds were characterized by Fourier transform infrared spectroscopy, electrospray ionization mass spectrometry, elemental analysis and nuclear magnetic resonance spectroscopy (NMR). They were heterogenized on commercially available activated carbon (AC) and multi-walled carbon nanotubes (CNT), as well as on their chemically modified analogues. The obtained materials were characterized by scanning electron microscopy, transmission electron microscopy and X-ray photoelectron spectroscopy. Complex 3 supported on activated carbon (3-AC) was found to be an active and recyclable catalyst for the cyanosilylation of several aromatic and aliphatic aldehydes. Using 3-AC with a low loading of 0.1 mol% several substrates were quantitatively converted, within just 5 min at 50 °C and under microwave irradiation in solvent-free conditions. Multinuclear NMR analysis suggested a mechanism that potentially involves a double activation process, where the nucleophilic phosphorus at the PTA derivative acts as a Lewis base and the Sn(IV) metal centre as a Lewis acid.publishersversionpublishe
Human gut symbiont Roseburia hominis promotes and regulates innate immunity
© 2017 Patterson, Mulder, Travis, Lan, Cerf-Bensussan, Gaboriau-Routhiau, Garden, Logan, Delday, Coutts, Monnais, Ferraria, Inoue, Grant and Aminov. Objective: Roseburia hominis is a flagellated gut anaerobic bacterium belonging to the Lachnospiraceae family within the Firmicutes phylum. A significant decrease of R. hominis colonization in the gut of ulcerative colitis patients has recently been demonstrated. In this work, we have investigated the mechanisms of R. hominis-host cross talk using both murine and in vitro models. Design: The complete genome sequence of R. hominis A2-183 was determined. C3H/HeN germ-free mice were mono-colonized with R. hominis, and the host-microbe interaction was studied using histology, transcriptome analyses and FACS. Further investigations were performed in vitro and using the TLR5KO and DSS-colitis murine models. Results: In the bacterium, R. hominis, host gut colonization upregulated genes involved in conjugation/mobilization, metabolism, motility, and chemotaxis. In the host cells, bacterial colonization upregulated genes related to antimicrobial peptides, gut barrier function, toll-like receptors (TLR) signaling, and T cell biology. CD4 + CD25 + FoxP3 + T cell numbers increased in the lamina propria of both mono-associated and conventional mice treated with R. hominis. Treatment with the R. hominis bacterium provided protection against DSS-induced colitis. The role of flagellin in host-bacterium interaction was also investigated. Conclusion: Mono-association of mice with R. hominis bacteria results in specific bidirectional gene expression patterns. A set of genes thought to be important for host colonization are induced in R. hominis, while the host cells respond by strengthening gut barrier function and enhancing Treg population expansion, possibly via TLR5-flagellin signaling. Our data reveal the immunomodulatory properties of R. hominis that could be useful for the control and treatment of gut inflammation
Measurement of the cross-section for b-jets produced in association with a Z boson at root s=7 TeV with the ATLAS detector ATLAS Collaboration
A measurement is presented of the inclusive cross-section for b-jet production in association with a Z boson in pp collisions at a centre-of-mass energy of root s = 7 TeV. The analysis uses the data sample collected by the ATLAS experiment in 2010, corresponding to an integrated luminosity of approximately 36 pb(-1). The event selection requires a Z boson decaying into high P-T electrons or muons, and at least one b-jet, identified by its displaced vertex, with transverse momentum p(T) > 25 GeV and rapidity vertical bar y vertical bar < 2.1. After subtraction of background processes, the yield is extracted from the vertex mass distribution of the candidate b-jets. The ratio of this cross-section to the inclusive Z cross-section (the average number of b-jets per Z event) is also measured. Both results are found to be in good agreement with perturbative QCD predictions at next-to-leading order
Beam-induced and cosmic-ray backgrounds observed in the ATLAS detector during the LHC 2012 proton-proton running period
This paper discusses various observations on beam-induced and cosmic-ray backgrounds in the ATLAS detector during the LHC 2012 proton-proton run. Building on published results based on 2011 data, the correlations between background and residual pressure of the beam vacuum are revisited. Ghost charge evolution over 2012 and its role for backgrounds are evaluated. New methods to monitor ghost charge with beam-gas rates are presented and observations of LHC abort gap population by ghost charge are discussed in detail. Fake jets from colliding bunches and from ghost charge are analysed with improved methods, showing that ghost charge in individual radio-frequency buckets of the LHC can be resolved. Some results of two short periods of dedicated cosmic-ray background data-taking are shown; in particular cosmic-ray muon induced fake jet rates are compared to Monte Carlo simulations and to the fake jet rates from beam background. A thorough analysis of a particular LHC fill, where abnormally high background was observed, is presented. Correlations between backgrounds and beam intensity losses in special fills with very high β* are studied
Beam-induced and cosmic-ray backgrounds observed in the ATLAS detector during the LHC 2012 proton-proton running period
This paper discusses various observations on beam-induced and cosmic-ray backgrounds
in the ATLAS detector during the LHC 2012 proton-proton run. Building on published
results based on 2011 data, the correlations between background and residual pressure of the beam
vacuum are revisited. Ghost charge evolution over 2012 and its role for backgrounds are evaluated.
New methods to monitor ghost charge with beam-gas rates are presented and observations of LHC
abort gap population by ghost charge are discussed in detail. Fake jets from colliding bunches and
from ghost charge are analysed with improved methods, showing that ghost charge in individual
radio-frequency buckets of the LHC can be resolved. Some results of two short periods of dedicated
cosmic-ray background data-taking are shown; in particular cosmic-ray muon induced fake jet rates
are compared to Monte Carlo simulations and to the fake jet rates from beam background. A
thorough analysis of a particular LHC fill, where abnormally high background was observed, is
presented. Correlations between backgrounds and beam intensity losses in special fills with very
high β∗ are studied
Electronic and optical sources of information for the humanities: a survey of library users, products and projects in Italy
Agli inizi degli anni 90, prima della diffusione del Web, le banche dati (e soprattutto le banche dati umanistiche)costituivano una realtà scarsamente conosciuta
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