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1.
J Phys Condens Matter ; 33(34)2021 Jul 01.
Article in English | MEDLINE | ID: mdl-34098548

ABSTRACT

Lithium-sulfur batteries are considered one of the possible next-generation energy-storage solutions, but to be commercially available many drawbacks have yet to be solved. One solution with great potentiality is the use of lithium sulfide as cathode material since it can be coupled to Li-free anodes, such as graphite, Si or Sn. Nevertheless, Li2S, like sulfur, is electronically and ionically insulating, with a high activation potential for its initial oxidation step. To overcome this issue, different strategies have been explored, one of them being the use of catalytic surfaces. In the present article, we study using first principles calculations the effect of the dielectric constant of the solvent on the activation energy of the cleavage reaction of Li2S on different catalytic surfaces. To the best of our knowledge, this is the first time that such a study is undertaken. We find that the effect of the solvent should be twofold: on one side, it should decrease the interaction between the Li2S molecule and the surface. On the other side, since the species arising in the dissociation reaction are charged, the solvent should decrease the activation barrier for the dissociation of the Li2S molecule, when compared with the reaction in vacuum. These theoretical findings are discussed in connection with experimental results from the literature, where the behaviour of the Li-S cathode is studied in different solvents.

2.
Phys Chem Chem Phys ; 23(5): 3281-3289, 2021 Feb 07.
Article in English | MEDLINE | ID: mdl-33506828

ABSTRACT

Complex materials composed of two and three elements with high Li-ion storage capacity are investigated and tested as lithium-ion battery (LiB) negative electrodes. Namely, anodes containing tin, silicon, and graphite show very good performance because of the large gravimetric and volumetric capacity of silicon and structural support provided by tin and graphite. The performance of the composites during the first cycles was studied using ex situ magic angle spinning (MAS) 7Li Nuclear Magnetic Resonance (NMR), density functional theory (DFT) calculations, and electrochemical techniques. The best performance was obtained for Sn/Si/graphite in a 1 : 1 : 1 proportion, due to an emergent effect of the interaction between Sn and Si. The results suggest a stabilization effect of Sn over Si, providing a physical constraint that prevents Si pulverization. This mechanism ensures good cyclability over more than one hundred cycles, low capacity fading and high specific capacity.

3.
Anal Chim Acta ; 596(2): 183-94, 2007 Jul 23.
Article in English | MEDLINE | ID: mdl-17631096

ABSTRACT

This work reports the advantages of using glassy carbon electrodes (GCEs) modified with multi-wall carbon nanotubes (CNT) dispersed in polyethylenimine (PEI) as detectors in flow injection and capillary electrophoresis. The presence of the dispersion of CNT in PEI at the electrode surface allows the highly sensitive and reproducible determination of hydrogen peroxide, different neurotransmitters (dopamine (D) and its metabolite dopac, epinephrine (E), norepinephrine (NE)), phenolic compounds (phenol (P), 3-chlorophenol (3-CP) and 2,3-dichlorophenol (2,3CP)) and herbicides (amitrol). Sensitivities enhancements of 150 and 140 folds compared to GCE were observed for hydrogen peroxide and amitrol, respectively. One of the most remarkable properties of the resulting electrode is the antifouling effect of the CNT/PEI layer. No passivation was observed either for successive additions (30) or continuous flow (for 30 min) of the compounds under investigation, even dopac or phenol. A critical comparison of the amperometric and voltammetric signal of these different analytes at bare- and PEI-modified glassy carbon electrodes and pyrolytic graphite electrodes is also included, demonstrating that the superior performance of CNT is mainly due to their unique electrochemical properties. Glassy carbon electrodes modified with CNT-PEI dispersion also show an excellent performance as amperometric detector in the electrophoretic separation of phenolic compounds and neurotransmitters making possible highly sensitive and reproducible determinations.

4.
Talanta ; 71(3): 1282-7, 2007 Feb 28.
Article in English | MEDLINE | ID: mdl-19071446

ABSTRACT

This work reports on the analytical performance of composites obtained by dispersing copper microparticles and multi-wall carbon nanotubes within a mineral oil binder (CNTPE-Cu) for the determination of amino acids and albumin. The strong complexing activity of amino acids towards copper makes possible an important improvement in the sensitivity for the determination of amino acids and albumin. This new electrode permits the highly sensitive amperometric detection of amino acids, even the non-electroactive ones, at very low potentials (0.000V) and physiological pH (phosphate buffer solution pH 7.40). The response of the electrode is highly dependent on the amount of copper, demonstrating the crucial role of the metal in the analytical performance of the sensor. The best analytical performance is obtained for the electrode containing 6.0% (w/w) copper. The resulting sensor shows a fast response (7s) and a sensitivity that depends on the nature of the amino acid. The electrode surface demonstrates an excellent resistance to surface fouling, with R.S.D. of 4% for the sensitivities of 10 successive calibration plots. Albumin is determined with CNTPE-Cu using a protocol based on the accumulation of the protein for 10min at -0.100V, followed by the square-wave voltammetric analysis. The quantification of albumin concentration in lyophilized control serum gives excellent agreement with the classical spectrophotometric methodology and with the value informed for the supplier.

5.
Talanta ; 74(3): 291-307, 2007 Dec 15.
Article in English | MEDLINE | ID: mdl-18371643

ABSTRACT

The aim of this review is to summarize the most relevant contributions in the development of electrochemical (bio)sensors based on carbon nanotubes in the last years. Since the first application of carbon nanotubes in the preparation of an electrochemical sensor, an increasing number of publications involving carbon nanotubes-based sensors have been reported, demonstrating that the particular structure of carbon nanotubes and their unique properties make them a very attractive material for the design of electrochemical biosensors. The advantages of carbon nanotubes to promote different electron transfer reactions, in special those related to biomolecules; the different strategies for constructing carbon nanotubes-based electrochemical sensors, their analytical performance and future prospects are discussed in this article.


Subject(s)
Biosensing Techniques/instrumentation , Nanotubes, Carbon/chemistry , Animals , DNA/analysis , DNA/chemistry , Electrochemistry , Electrodes , Humans
6.
Anal Chim Acta ; 577(2): 183-9, 2006 Sep 08.
Article in English | MEDLINE | ID: mdl-17723670

ABSTRACT

In this work we report on the successful use of a composite prepared by dispersion of multi-wall carbon nanotubes (1-5 microm length, 20-50 nm diameter) and copper microparticles within mineral oil as detector for amino acids quantification in flow injection analysis and capillary electrophoresis. The resulting electrode displays a highly sensitive amperometric detection of amino acids, based on the copper dissolution facilitated by the strong activity of amino acids as ligands of Cu(II). The sensor makes possible the detection of amino acids, electroactive or not, at very low potentials (0.000 V) and physiological pH. A correlation between the sensitivity for the amino acids and the amount of copper within the composite is observed, demonstrating the importance of the metal in the sensor response. The best analytical performance is obtained for the electrode containing 12.0% (w/w) copper. The excellent results obtained with the carbon nanotube paste electrodes containing copper (CNTPE-Cu) as detector in flow systems makes them an interesting alternative for further analytical applications involving different bioanalytes.

7.
Talanta ; 66(2): 467-71, 2005 Apr 15.
Article in English | MEDLINE | ID: mdl-18970008

ABSTRACT

The performance of amperometric glucose biosensors based on the dispersion of glucose oxidase (GOx) and copper oxide within a classical carbon (graphite) paste composite is reported in this work. Copper oxide promotes an excellent electrocatalytic activity towards the oxidation and reduction of hydrogen peroxide, allowing a large decrease in the oxidation and reduction overpotentials, as well as an important enhancement of the corresponding currents. Therefore, it is possible to perform the glucose biosensing at low potentials where there is no interference even in large excess of ascorbic acid, uric acid or acetaminophen. The influence of the copper oxide and glucose oxidase content in the paste on the analytical performance of the bioelectrode is discussed. The resulting biosensor shows a fast response, a linear relationship between current and glucose concentration up to 1.35 x 10(-2) M (2.43 g L(-1)) and a detection limit of 2.0 x 10(-5) M. The effect of the presence of the enzyme in the composite material on the dispersion of the copper oxide particles is also discussed.

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