22 research outputs found

    Fast Ionic Conductivity in the Most Lithium-Rich Phosphidosilicate Li14SiP6.

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    Solid electrolytes with superionic conductivity are required as a main component for all-solid-state batteries. Here we present a novel solid electrolyte with three-dimensional conducting pathways based on "lithium-rich" phosphidosilicates with ionic conductivity of σ > 10-3 S cm-1 at room temperature and activation energy of 30-32 kJ mol-1 expanding the recently introduced family of lithium phosphidotetrelates. Aiming toward higher lithium ion conductivities, systematic investigations of lithium phosphidosilicates gave access to the so far lithium-richest compound within this class of materials. The crystalline material (space group Fm3m), which shows reversible thermal phase transitions, can be readily obtained by ball mill synthesis from the elements followed by moderate thermal treatment of the mixture. Lithium diffusion pathways via both tetrahedral and octahedral voids are analyzed by temperature-dependent powder neutron diffraction measurements in combination with maximum entropy method and DFT calculations. Moreover, the lithium ion mobility structurally indicated by a disordered Li/Si occupancy in the tetrahedral voids plus partially filled octahedral voids is studied by temperature-dependent impedance and 7Li NMR spectroscopy

    Dielectric signature of charge order in lanthanum nickelates

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    Three charge-ordering lanthanum nickelates La2-xAxNiO4, substituted with specific amounts of A = Sr, Ca, and Ba to achieve commensurate charge order, are investigated using broadband dielectric spectroscopy up to GHz frequencies. The transition temperatures of the samples are characterized by additional specific heat and magnetic susceptibility measurements. We find colossal magnitudes of the dielectric constant for all three compounds and strong relaxation features, which partly are of Maxwell-Wagner type arising from electrode polarization. Quite unexpectedly, the temperature-dependent colossal dielectric constants of these materials exhibit distinct anomalies at the charge-order transitions.Comment: 7 pages, 6 figure

    Latest developments in non-faradic impedimetric biosensors: Towards clinical applications

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    The field of capacitive biosensors has grown significantly since the last comprehensive assessment by Daniels et al. in 2007. Here we how new trends in molecular imprinting, nanotechnology and microfluidics are now being exploited and demonstrate how capacitive biosensors are on the verge of becoming clinically relevant. We also shed light on recent developments in terms of test-setup, surface chemistry and test solutions

    Fast Lithium ion conduction in Lithium phosphidoaluminates

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    Solid electrolyte materials are crucial for the development of high‐energy‐density all‐solid‐state batteries (ASSB) using a nonflammable electrolyte. In order to retain a low lithium‐ion transfer resistance, fast lithium ion conducting solid electrolytes are required. We report on the novel superionic conductor Li9AlP4 which is easily synthesised from the elements via ball‐milling and subsequent annealing at moderate temperatures and which is characterized by single‐crystal and powder X‐ray diffraction. This representative of the novel compound class of lithium phosphidoaluminates has, as an undoped material, a remarkable fast ionic conductivity of 3 mS cm−1 and a low activation energy of 29 kJ mol−1 as determined by impedance spectroscopy. Temperature‐dependent 7Li NMR spectroscopy supports the fast lithium motion. In addition, Li9AlP4 combines a very high lithium content with a very low theoretical density of 1.703 g cm−3. The distribution of the Li atoms over the diverse crystallographic positions between the [AlP4]9− tetrahedra is analyzed by means of DFT calculations

    A graphene-based pH sensor on paper for human plasma and seawater

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    The relevance of pH assessment in clinical analysis, environmental and industrial control, has raised the demand for the development of portable, low cost and easy-to-use monitoring systems. This paper proposes a pH sensor printed on a paper support passivated with a solid-ink coating. The sensor exploits the pH sensitivity of a reduced graphene oxide functionalized with 3-(4-aminophenil)propionic acid. The sensor responded in the pH range [4, 10] and had a sensitivity of 46 mV/pH. Tests on human plasma and seawater proved this pH sensor to have similar performances than those of a commercial pH-meter with an uncertainty of 0.1 and 0.2 pH unit in plasma and seawater, respectively

    Advances in biosensing: The CRISPR/Cas system as a new powerful tool for the detection of nucleic acids

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    A main challenge in the development of biosensing devices for the identification and quantification of nucleic acids is to avoid the amplification of the genetic material from the sample by polymerase chain reaction (PCR), which is at present necessary to enhance sensitivity and selectivity of assays. PCR has undoubtedly revolutionized genetic analyses, but it requires careful purification procedures that are not easily implemented in point of care (POC) devices. In recent years, a new strategy for nucleic acid detection based on clustered regularly interspaced short palindromic repeats (CRISPR) and associated protein systems (Cas) seems to offer unprecedented possibilities. The coupling of the CRISPR/Cas system with recent isothermal amplification methods is fostering the development of innovative optical and electrochemical POC devices. In this review, the mechanisms of action of several new CRISRP/Cas systems are reported together with their use in biosensing of nucleic acids

    Biphenyl substituted lysine derivatives as recognition elements for the matrix metalloproteinases MMP-2 and MMP-9

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    Matrix metalloproteinases (MMPs) are an important factor in cancer progression and metastasis, especially gelatinases MMP-2 and MMP-9. A simple methodology for their detection and monitoring is highly desirable. Molecular probes have been very widely and successfully applied to study the activity of MMPs in cellular processes in vitro. We thus synthesized a small compound library of MMP-2 and MMP-9 binding probes based on drug molecules and endowed with free amine groups for the functionalization of transducer surfaces. In this study, we combined experimental results obtained by a kinetic fluorogenic peptide substrate cleavage assay with molecular modeling studies in order to assess the ability of the probe to bind to their target enzymes. The synthesized biphenyl substituted lysine derivatives showed IC50-values in the low nanomolar concentration range against MMP-2 (ligands 3a-d: 3 nM to 8 ”M, ligands 4a-d: 45 nM to 350 ”M) and low micromolar range against MMP-9 (ligands 3a-d: 350 nM to 60 ”M, ligands 4a-d: 5 ”M to 600 ”M), with a selectivity up to more than 160-fold for MMP-2. The experimental results correlated well with molecular modelling with FleXAID and X-score functions. We showed that in our compound series, the side chain remained far away from the S1â€Č cavity and the ligand for all the docked minima. Ligands 4a-d with their free amine group on the side chain may thus be bound to transducer surfaces for the fabrication of sensors, while retaining their activity against their target enzymes

    Microbial biofilm monitoring by electrochemical transduction methods

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    The negative impact of biofilms in both the industry and the human health, demands the development of strategies for the in situ and early detection of biofilm formation. In this review we describe potentiometric, voltammetric and impedance-based sensors as to provide an overview of the different electrochemical techniques applied in biofilm detection and monitoring

    A Biosensor for the Detection of Acetylcholine and Diazinon

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    Acetylcholine is a neurotransmitter and a neuromodulator found in the autonomic, peripheral and central nervous systems. Diazinon is a pesticide with toxic effects on humans, such as the inhibition of acetylcholine. In this paper, a biosensor is proposed for the detection of acetylcholine (range 70 -1000 ΌΜ) and diazinon (range 0.3 -20000 ppb). This biosensor combines a pH-sensitive layer of reduced graphene oxide functionalized with 4-aminobenzoic acid and acetylcholinesterase. This enzyme was immobilized on reduced graphene oxide and it catalyzed the conversion of acetylcholine into choline and acetic acid, locally decreasing the pH value and triggering the sensor response. The limit of detection for the acetylcholine and diazinon were 70 ΌΜ and 0.3 ppb, respectively
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