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1.
ACS Appl Mater Interfaces ; 14(48): 53636-53647, 2022 Dec 07.
Article in English | MEDLINE | ID: mdl-36409931

ABSTRACT

Polymer electrolytes are attractive candidates to boost the application of rechargeable lithium metal batteries. Single-ion conducting polymers may reduce polarization and lithium dendrite growth, though these materials could be mechanically overly rigid, thus requiring ion mobilizers such as organic solvents to foster transport of Li ions. An inhomogeneous mobilizer distribution and occurrence of preferential Li transport pathways eventually yield favored spots for Li plating, thereby imposing additional mechanical stress and even premature cell short circuits. In this work, we explored ceramic-in-polymer hybrid electrolytes consisting of polymer blends of single-ion conducting polymer and PVdF-HFP, including EC/PC as swelling agents and silane-functionalized LATP particles. The hybrid electrolyte features an oxide-rich layer that notably stabilizes the interphase toward Li metal, enabling single-side lithium deposition for over 700 h at a current density of 0.1 mA cm-2. The incorporated oxide particles significantly reduce the natural solvent uptake from 140 to 38 wt % despite maintaining reasonably high ionic conductivities. Its electrochemical performance was evaluated in LiNi0.6Co0.2Mn0.2O2 (NMC622)||Li metal cells, exhibiting impressive capacity retention over 300 cycles. Notably, very thin LiNbO3 coating of the cathode material further boosts the cycling stability, resulting in an overall capacity retention of 78% over more than 600 cycles, clearly highlighting the potential of hybrid electrolyte concepts.

2.
J Family Med Prim Care ; 10(8): 3154-3158, 2021 Aug.
Article in English | MEDLINE | ID: mdl-34660462

ABSTRACT

INTRODUCTION: Budd-Chiari syndrome (BCS) is a rare condition affecting one in a million adults. BCS involves outflow obstruction in the hepatic venous system, which can occur anywhere between the small hepatic veins and the atrio-caval junction and cannot be due to heart, pericardial, or hepatic veno-occlusive disease. CASE PRESENTATION: We report an exceedingly rare form of BCS with less common initial clinical features in a young poor adult male patient which ignited a diagnostic uncertainty and a therapeutic challenge. The presence of the classical triad of BCS in the absence of major hepatic vein obstruction prompted the medical team to consider that the patient had a rare form of BCS. In this case, the financial condition of the patient and limited resources available restricted our ability to advance into the specific investigations. However, the patient was given symptomatic medical treatment and was followed up monthly. We also provided the patient with a statement that reaffirmed our inability to provide affordable surgical management options and called for an optimized national clinical guideline that could help the physicians deal with the challenges. CONCLUSION: An uncommon form of BCS in this patient provided a diagnostic challenge and therapeutic uncertainty in the low-resource settings. Primary care physicians should commence evidenced medical management based on clinical suspicion acknowledging the fact that obstruction of small hepatic veins is often not detected on an ultrasound.

3.
Materials (Basel) ; 14(13)2021 Jun 22.
Article in English | MEDLINE | ID: mdl-34206527

ABSTRACT

A spray-flame reaction step followed by a short 1-h sintering step under O2 atmosphere was used to synthesize nanocrystalline cubic Al-doped Li7La3Zr2O12 (LLZO). The as-synthesized nanoparticles from spray-flame synthesis consisted of the crystalline La2Zr2O7 (LZO) pyrochlore phase while Li was present on the nanoparticles' surface as amorphous carbonate. However, a short annealing step was sufficient to obtain phase pure cubic LLZO. To investigate whether the initial mixing of all cations is mandatory for synthesizing nanoparticulate cubic LLZO, we also synthesized Li free LZO and subsequently added different solid Li precursors before the annealing step. The resulting materials were all tetragonal LLZO (I41/acd) instead of the intended cubic phase, suggesting that an intimate intermixing of the Li precursor during the spray-flame synthesis is mandatory to form a nanoscale product. Based on these results, we propose a model to describe the spray-flame based synthesis process, considering the precipitation of LZO and the subsequent condensation of lithium carbonate on the particles' surface.

4.
Chem Sci ; 10(41): 9530-9541, 2019 Nov 07.
Article in English | MEDLINE | ID: mdl-32055324

ABSTRACT

In spite of achieving high power conversion efficiency (PCE), organo-halide perovskites suffer from long term stability issues. Especially the grain boundaries of polycrystalline perovskite films are considered as giant trapping sites for photo-generated carriers and therefore play an important role in charge transportation dynamics. Surface engineering via grain boundary modification is the most promising way to resolve this issue. A unique antisolvent-cum-quantum dot (QD) assisted grain boundary modification approach has been employed for creating monolithically grained, pin-hole free perovskite films, wherein the choice of all-inorganic CsPbBr x I3-x (x = 1-2) QDs is significant. The grain boundary filling by QDs facilitates the formation of compact films with 1-2 µm perovskite grains as compared to 300-500 nm grains in the unmodified films. The solar cells fabricated by CsPbBr1.5I1.5 QD modification yield a PCE of ∼16.5% as compared to ∼13% for the unmodified devices. X-ray photoelectron spectral analyses reveal that the sharing of electrons between the PbI6 - framework in the bulk perovskite and Br- ions in CsPbBr1.5I1.5 QDs facilitates the charge transfer process while femtosecond transient absorption spectroscopy (fs-TAS) suggests quicker trap filling and enhanced charge carrier recombination lifetime. Considerable ambient stability up to ∼720 h with <20% PCE degradation firmly establishes the strategic QD modification of bulk perovskite films.

5.
Langmuir ; 34(35): 10197-10216, 2018 09 04.
Article in English | MEDLINE | ID: mdl-29584956

ABSTRACT

The unique properties of II-VI semiconductor nanocrystals such as superior light absorption, size-dependent optoelectronic properties, solution processability, and interesting photophysics prompted quantum-dot-sensitized solar cells (QDSSCs) as promising candidates for next-generation photovoltaic (PV) technology. QDSSCs have advantages such as low-cost device fabrication, multiple exciton generation, and the possibility to push over the theoretical power conversion efficiency (PCE) limit of 32%. In spite of dedicated research efforts to enhance the PCE, optimize individual solar cell components, and better understand the underlying science, QDSSCs have unfortunately not lived up to their potential due to shortcomings in the fabrication process and with the QDs themselves. In this feature article, we briefly discuss the QDSSC concepts and mechanisms of the charge carrier recombination pathways that occur at multiple interfaces, viz., (i) metal oxide (MO)/QDs, (ii) MO/QDs/electrolyte, and (iii) counter electrode (CE)/electrolyte. The rational strategies that have been developed to minimize/block these charge recombination pathways are elaborated. The article concludes with a discussion of the present challenges in fabricating efficient devices and future prospects for QDSSCs.

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