Su Bin Park

In Operando Monitoring of the Pore Dynamics in Ordered Mesoporous Electrode Materials by Small Angle X-ray Scattering.

To monitor dynamic volume changes of electrode materials during electrochemical lithium storage and removal process is of utmost importance for developing high performance lithium storage materials. We herein report an in operando probing of mesoscopic structural changes in ordered mesoporous electrode materials during cycling with synchrotron-based small angel X-ray scattering (SAXS) technique. In operando SAXS studies combined with electrochemical and other physical characterizations straightforwardly show how porous electrode materials underwent volume changes during the whole process of charge and discharge, with respect to their own reaction mechanism with lithium. This comprehensive information on the pore dynamics as well as volume changes of the electrode materials will not only be critical in further understanding of lithium ion storage reaction mechanism of materials, but also enable the innovative design of high performance nanostructured materials for next generation batteries.

Highly Ordered Mesoporous WO3 with Excellent Catalytic Performance and Reusability for Deep Oxidative Desulfurization

Highly ordered mesoporous tungsten trioxide (WO3) with high surface area (75 m2/g) and well-defined mesopores were successfully prepared through a hard templating method using a mesoporous silica KIT-6 as a template and (NH4)6H2W12O40 ⋅ xH2O as a tungsten precursor. Oxidative desulfurization of a model oil with H2O2 as the oxidant was carried out at 50°C under atmospheric pressure in order to analyze the catalytic activity. The desulfurization reactions were optimized by various kinds of reaction parameters such as H2O2/S molar ratio, reaction temperatures and series of sulfur-containing compounds [dibenzothiophene (DBT), benzothiophene (BT) and 4,6-dimethyl dibenzothiophene (4,6-DMBT)]. Excellent catalytic activity for the removal of the sulfur-containing compounds from the model oil was observed with mesoporous WO3 catalyst, where the activity was maintained during 5 recycle tests without any regeneration process. The high catalytic activity and durability is mainly attributed to well-defined mesopores and high surface area of mesoporous WO3 catalyst.

Exceptional Lithium Storage in a Co(OH)2 Anode: Hydride Formation

Current lithium ion battery technology is tied in with conventional reaction mechanisms such as insertion, conversion, and alloying reactions even though most future applications like EVs demand much higher energy densities than current ones. Exploring the exceptional reaction mechanism and related electrode materials can be critical for pushing current battery technology to a next level. Here, we introduce an exceptional reaction with a Co(OH)2 material which exhibits an initial charge capacity of 1112 mAh g-1, about twice its theoretical value based on known conventional conversion reaction, and retains its first cycle capacity after 30 cycles. The combined results of synchrotron X-ray diffraction and X-ray absorption spectroscopy indicate that nanosized Co metal particles and LiOH are generated by conversion reaction at high voltages, and Co xH y, Li2O, and LiH are subsequently formed by hydride reaction between Co metal, LiOH, and other lithium species at low voltages, resulting in a anomalously high capacity beyond the theoretical capacity of Co(OH)2. This is further corroborated by AIMD simulations, localized STEM, and XPS. These findings will provide not only further understanding of exceptional lithium storage of recent nanostructured materials but also valuable guidance to develop advanced electrode materials with high energy density for next-generation batteries.

Nanostructural Uniformity of Ordered Mesoporous Materials: Governing Lithium Storage Behaviors

Nanostructured materials make a considerable impact on the performance of lithium-storage characteristics in terms of the energy density, power density, and cycle life. Direct experimental observation, by a comparison of controlled nanostructural uniformity of electrode materials, reveals that the lithium-storage behaviors of mesoporous MoO2 and CuO electrodes are linearly correlated with their nanostructural uniformity. Reversible capacities of mesoporous MoO2 and CuO electrodes with well-developed nanostructures (1569 mA h g-1 for MoO2 and 1029 mA h g-1 for CuO) exceed their theoretical capacity based on the conversion reaction (838 mA h g-1 for MoO2 and 674 mA h g-1 for CuO). Given that exact understanding of the origin of the additional capacity is essential in maximizing the energy density of electrode material, this work may help to gain some insights into the development of high energy-density lithium-storage materials for next-generation lithium rechargeable batteries.