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Ultrathin two-dimensional conjugated metal– organic framework single-crystalline nanosheets enabled by surfactant-assisted synthesis
Two-dimensional conjugated metal-organic frameworks (2D c-MOFs) have recently emerged for potential applications in (opto-)electronics, chemiresistive sensing, and energy storage and conversion, due to their excellent electrical conductivity, abundant active sites, and intrinsic porous structures. However, developing ultrathin 2D c-MOF nanosheets (NSs) for facile solution processing and integration into devices remains a great challenge, mostly due to unscalable synthesis, low yield, limited lateral size and low crystallinity. Here, we report a surfactant-assisted solution synthesis toward ultrathin 2D c-MOF NSs, including HHB-Cu (HHB = hexahydroxybenzene), HHB-Ni and HHTP-Cu (HHTP = 2,3,6,7,10,11-hexahydroxytriphenylene). For the first time, we achieve single-crystalline HHB-Cu(Ni) NSs featured with a thickness of 4-5 nm (∼8-10 layers) and a lateral size of 0.25-0.65 μm2, as well as single-crystalline HHTP-Cu NSs with a thickness of ∼5.1 ± 2.6 nm (∼10 layers) and a lateral size of 0.002-0.02 μm2. Benefiting from the ultrathin feature, the synthetic NSs allow fast ion diffusion and high utilization of active sites. As a proof of concept, when serving as a cathode material for Li-ion storage, HHB-Cu NSs deliver a remarkable rate capability (charge within 3 min) and long-term cycling stability (90% capacity retention after 1000 cycles), superior to the corresponding bulk materials and other reported MOF cathodes. This journal is © The Royal Society of Chemistry.
Investigating the electrochemical stability of Li7La3Zr2O12 solid electrolytes using field stress experiments
Cubic Li7La3Zr2O12 (LLZO) garnets are among the most promising solid electrolytes for solid-state batteries with the potential to exceed conventional battery concepts in terms of energy density and safety. The electrochemical stability of LLZO is crucial for its application, however, controversial reports in the literature show that it is still an unsettled matter. Here, we investigate the electrochemical stability of LLZO single crystals by applying electric field stress via macro- and microscopic ionically blocking Au electrodes in ambient air. Induced material changes are subsequently probed using various locally resolved analysis techniques, including microelectrode electrochemical impedance spectroscopy (EIS), laser induced breakdown spectroscopy (LIBS), laser ablation-inductively coupled plasma-mass spectrometry (LA-ICP-MS), and microfocus X-ray diffraction (XRD). Our experiments indicate that LLZO decomposes at 4.1–4.3 V vs. Li+/Li, leading to the formation of Li-poor phases like La2Zr2O7 beneath the positively polarized electrode. The reaction is still on-going even after several days of polarization, indicating that no blocking interfacial layer is formed. The decomposition can be observed at elevated as well as room temperature and suggests that LLZO is truly not compatible with high voltage cathode materials.
Cathode fall voltage of TIG arcs from a non-equilibrium arc model
This work presents modelling results concerning a tungsten inert gas (TIG) welding arc. The model provides a consistent description of the free burning arc, the arc attachment and the electrodes. Thermal and chemical non-equilibrium is considered in the whole arc area, and a detailed model of the cathode space-charge sheath is included. The mechanisms in the cathode pre-sheath are treated in the framework of a non-equilibrium approach which is based on a two-fluid description of electrons and heavy particles and a simplified plasma chemistry of argon. A consistent determination of the electrode fall voltages and temperature distributions is achieved. The model is applied to arcs in pure argon at currents up to 250 A, whereby welding of a workpiece made of mild steel with a fixed burner is considered. Arc voltages in the range from 12 to 17 V are obtained at 50 at 250 A, respectively. The space-charge sheath voltage is found to be about 7 V and almost independent of the current. The corresponding temperatures of the cathode tip are in the range from 3,000 K to about 3,800 K. The results obtained are in a good agreement with measurements.