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Author ORCID ID is 0000000280463931
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  1. We examined the electrosorption and ion dynamics of imidazolium-based room temperature ionic liquids (RTILs) having short (3-carbon, C3mim +) and long (12-carbon, C12mim +) cations, that is, 1-propyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (C3mimTFSI) and 1-dodecyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (C12mimTFSI), confined in ordered mesoporous carbon (OMC) and analyzed the influence of the cation alkyl chain length on the ion dynamics and the capacitive behavior using electrochemical measurements together with quasi-elastic neutron scattering (QENS) observations and classical density functional theory (cDFT) computations. Electrochemical tests highlighted the significant influence of specific applied potentials on accumulated charge storage densities and on the limits of saturation of larger electrolytes inmore » the pores. Computational analyses corroborated these findings and predicted a 16% increase in the capacitance of the smaller-cation electrolyte under high applied potentials. However, QENS experiments revealed a behavior of decoupling of alkyl chain dynamics from the ring in electrolytes with larger ions. cDFT calculations identified density spikes for C12mim + away from the pore walls to further corroborate this unique behavior. Here, our insights into chain length-dependent dynamics and electrosorption in complex electrolyte-electrode systems deepen fundamental understanding of confined RTIL electrolyte behavior in the porous carbon electrodes.« less
  2. A dual-template strategy for facile preparation of a bifunctional oxygen electrocatalyst for high-performance rechargeable zinc–air batteries has been reported.
  3. Zeolite materials play a significant role throughout the oil refining and petrochemical industry. Microporous ZSM-5 has a high degree of crystallinity but low mass transfer, while hierarchical ZSM-5 shows a low degree of crystallinity as well as acidity. Here, we first report the synthesis of ZSM-5 with a new morphological structure, which has nanocrystalline ZSM-5 particles on the surface of an intact ZSM-5 zeolite. This not only improved the mass transfer in microporosity but also overcame disadvantages of hierarchical ZSM-5 including low degrees of crystallinity and acidity. This new and very efficient structure with both intracrystal microporosity and intercrystal macroporosity,more » formed by secondary crystallization after the intact ZSM-5 zeolite was synthesized, was verified by transmission electronic microscopy, N 2 adsorption and desorption, and X-ray diffraction. Lastly, the obtained ZSM-5 zeolite showed a uniform size (~200 nm), high crystallinity acidity, and a suitable hierarchical structure that exhibited excellent properties in the catalytic fast pyrolysis of cellulose to produce aromatics.« less
  4. Tin and tin oxide-based electrodes are promising high-capacity anodes for lithium-ion batteries. However, poor capacity retention is the major issue with these materials due to the large volumetric expansion that occurs when lithium is alloyed with tin during lithiation and delithiation process. Here, a method to prepare a low-cost, scalable carbon and tin(II) oxide composite anode is reported. The composite material was prepared by ball milling of carbon recovered from used tire powders with 25 wt% tin(II) oxide to form lithium-ion battery anode. With the impact of energy from the ball milling, tin oxide powders were uniformly distributed inside themore » pores of waste-tire-derived carbon. During lithiation and delithiation, the carbon matrix can effectively absorb the volume expansion caused by tin, thereby minimizing pulverization and capacity fade of the electrodes. In conclusion, the as-synthesized anode yielded a capacity of 690 mAh g –1 after 300 cycles at a current density of 40 mA g –1 with a stable battery performance.« less
  5. The porous liquid zeolites with permanent porosity could be fabricated by exploiting the hydrogen bonding interaction between the alkane chains of branched ionic liquids and the Brønsted sites in H-form zeolites.
  6. Achieving homogeneous dispersion of nanoporous fillers within membrane architectures remains a great challenge for mixed-matrix membrane (MMMs) technology. Imparting solution processability of nanoporous materials would help advance the development of MMMs for membrane-based gas separations. A mechanochemically assisted oxidative coupling polymerization strategy was used to create a new family of soluble nanoporous polymer networks. The solid-state ball-milling method affords inherent molecular weight control over polymer growth and therefore provides unexpected solubility for the resulting nanoporous frameworks. MMM-based CO 2/CH 4 separation performance was significantly accelerated by these new soluble fillers. In conclusion, we anticipate this facile method will facilitate newmore » possibilities for the rational design and synthesis of soluble nanoporous polymer networks and promote their applications in membrane-based gas separations.« less
  7. A star-shape polymer of 3-armed poly(ethylene glycol) methyl ether methacrylate-co-glycidyl methacrylate copolymer (3PPEGM-co-GMA) was synthesized using an atom transfer radical polymerization (ATRP) technique. All-solid-state interpenetrating network polymer electrolytes (INSPEs) were fabricated by simultaneous reaction of 3PPEGM-co-GMA and bisphenol A diglycidyl ether (BPDE) with polyetherdiamine (ED2003) in the presence of lithium bis(trifluoromethane) sulfonamide (LiTFSI). The INSPEs exhibited ionic conductivities higher than 10 -5 S cm -1 at room temperature, a high oxidation stability of 4.5 vs. Li/Li + and remarkable stability towards lithium metal. Li metal batteries with LiFePO 4 as the cathode and INSPEs as the electrolyte cycled at amore » current rate of 0.1C at 60 °C showed a high initial discharge capacity of 156.2 mA h g -1 and a stable cycling performance over 200 cycles with a high coulombic efficiency of 99%. In conclusion, the results demonstrate that the interpenetrating network polymer electrolytes are promising electrolytes for next generation lithium-based batteries with high ionic conductivity, improved safety, and stable electrochemical performance.« less
  8. The poor water stability of most porous coordination polymers (PCPs) or metal-organic frameworks (MOFs) is widely recognised as a barrier hampering their practical applications. Herein, a facile and scalable route to prepare metal-containing polymers with a good stability in boiling water (100°C, 24 h) and air (up to 390°C) is presented. The bifunctional 1-vinylimidazole (VIm) with both a coordinating site and a polymerizable organic group is introduced as the building block. This core strategy includes the synthesis of a rigid monomer with four VIm branches via a coordination process at room temperature, followed by a radical polymerization. Here we callmore » this material Coordination-supported Imidazolate Networks (CINs). Interestingly, CINs are composed of rich mesopores from 2 to 15 nm, as characterized by low-energy (60 kV) STEM-HAADF images. Especially, the stable CINs illustrate a high turnover frequency (TOF) of 779 h -1 in the catalytic oxidation of phenol with H 2O as the green solvent.« less

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