Ki-Joon Jeon

Air-stable magnesium nanocomposites provide rapid and high-capacity hydrogen storage without using heavy-metal catalysts

Hydrogen is a promising alternative energy carrier that can potentially facilitate the transition from fossil fuels to sources of clean energy because of its prominent advantages such as high energy density (142 MJ kg(-1); ref. 1), great variety of potential sources (for example water, biomass, organic matter), light weight, and low environmental impact (water is the sole combustion product). However, there remains a challenge to produce a material capable of simultaneously optimizing two conflicting criteria--absorbing hydrogen strongly enough to form a stable thermodynamic state, but weakly enough to release it on-demand with a small temperature rise. Many materials under development, including metal-organic frameworks, nanoporous polymers, and other carbon-based materials, physisorb only a small amount of hydrogen (typically 1-2 wt%) at room temperature. Metal hydrides were traditionally thought to be unsuitable materials because of their high bond formation enthalpies (for example MgH(2) has a ΔHf~75 kJ mol(-1)), thus requiring unacceptably high release temperatures resulting in low energy efficiency. However, recent theoretical calculations and metal-catalysed thin-film studies have shown that microstructuring of these materials can enhance the kinetics by decreasing diffusion path lengths for hydrogen and decreasing the required thickness of the poorly permeable hydride layer that forms during absorption. Here, we report the synthesis of an air-stable composite material that consists of metallic Mg nanocrystals (NCs) in a gas-barrier polymer matrix that enables both the storage of a high density of hydrogen (up to 6 wt% of Mg, 4 wt% for the composite) and rapid kinetics (loading in <30 min at 200 °C). Moreover, nanostructuring of the Mg provides rapid storage kinetics without using expensive heavy-metal catalysts.

Fluorographene: A Wide Bandgap Semiconductor with Ultraviolet Luminescence

The manipulation of the bandgap of graphene by various means has stirred great interest for potential applications. Here we show that treatment of graphene with xenon difluoride produces a partially fluorinated graphene (fluorographene) with covalent C-F bonding and local sp(3)-carbon hybridization. The material was characterized by Fourier transform infrared spectroscopy, Raman spectroscopy, electron energy loss spectroscopy, photoluminescence spectroscopy, and near edge X-ray absorption spectroscopy. These results confirm the structural features of the fluorographane with a bandgap of 3.8 eV, close to that calculated for fluorinated single layer graphene, (CF)(n). The material luminesces broadly in the UV and visible light regions, and has optical properties resembling diamond, with both excitonic and direct optical absorption and emission features. These results suggest the use of fluorographane as a new, readily prepared material for electronic, optoelectronic applications, and energy harvesting applications.

The Interaction of Li+ with Single-Layer and Few-Layer Graphene

The interaction of Li(+) with single and few layer graphene is reported. In situ Raman spectra were collected during the electrochemical lithiation of the single- and few-layer graphene. While the interaction of lithium with few layer graphene seems to resemble that of graphite, single layer graphene behaves very differently. The amount of lithium absorbed on single layer graphene seems to be greatly reduced due to repulsion forces between Li(+) at both sides of the graphene layer.

Enhanced Nanoscale Friction on Fluorinated Graphene

Atomically thin graphene is an ideal model system for studying nanoscale friction due to its intrinsic two-dimensional (2D) anisotropy. Furthermore, modulating its tribological properties could be an important milestone for graphene-based micro- and nanomechanical devices. Here, we report unexpectedly enhanced nanoscale friction on chemically modified graphene and a relevant theoretical analysis associated with flexural phonons. Ultrahigh vacuum friction force microscopy measurements show that nanoscale friction on the graphene surface increases by a factor of 6 after fluorination of the surface, while the adhesion force is slightly reduced. Density functional theory calculations show that the out-of-plane bending stiffness of graphene increases up to 4-fold after fluorination. Thus, the less compliant F-graphene exhibits more friction. This indicates that the mechanics of tip-to-graphene nanoscale friction would be characteristically different from that of conventional solid-on-solid contact and would be dominated by the out-of-plane bending stiffness of the chemically modified graphene. We propose that damping via flexural phonons could be a main source for frictional energy dissipation in 2D systems such as graphene.

Direct Imaging of Soft-Hard Interfaces Enabled by Graphene

Direct imaging of surface molecules and the interfaces between soft and hard materials on functionalized nanoparticles is a great challenge using modern microscopy techniques. We show that graphene, a single atomic layer of sp(2)-bonded carbon atoms, can be employed as an ultrathin support film that enables direct imaging of molecular layers and interfaces in both conventional and atomic-resolution transmission electron microscopy. An atomic-resolution imaging study of the capping layers and interfaces of citrate-stabilized gold nanoparticles is used to demonstrate this novel capability. Our findings reveal the unique potential of graphene as an ideal support film for atomic-resolution transmission electron microscopy of hard and soft nanomaterials.

Highly p-doped epitaxial graphene obtained by fluorine intercalation

We present a method for decoupling epitaxial graphene grown on SiC(0001) by intercalation of a layer of fluorine at the interface. The fluorine atoms do not enter into a covalent bond with graphene but rather saturate the substrate Si bonds. This configuration of the fluorine atoms induces a remarkably large hole density of p≈4.5×1013 cm−2, equivalent to the location of the Fermi level at 0.79 eV above the Dirac point ED.

Silicon Diphosphide: A Si-Based Three-Dimensional Crystalline Framework as a High-Performance Li-Ion Battery Anode

The development of an electrode material for rechargeable Li-ion batteries (LIBs) and the understanding of its reaction mechanism play key roles in enhancing the electrochemical characteristics of LIBs for use in various portable electronics and electric vehicles. Here, we report a three-dimensional (3D) crystalline-framework-structured silicon diphosphide (SiP2) and its interesting electrochemical behaviors for superior LIBs. During Li insertion in the SiP2, a three-step electrochemical reaction mechanism, sequentially comprised of a topotactic transition (0.55-2 V), an amorphization (0.25-2 V), and a conversion (0-2 V), was thoroughly analyzed. On the basis of the three-step electrochemical reaction mechanism, excellent electrochemical properties, such as high initial capacities, high initial Coulombic efficiencies, stable cycle behaviors, and fast-rate capabilities, were attained from the preparation of a nanostructured SiP2/C composite. This 3D crystalline-framework-structured SiP2 compound will be a promising alternative anode material in the realization and mass production of excellent, rechargeable LIBs.

A Simulation Study on the Collection of Submicron Particles in a Unipolar Charged Fiber

In this study, we developed a simulation method to predict the initial collection efficiency of a unipolar charged fiber and the particle deposition morphology in the electret filter composed of unipolar charged fibers. The particle sizes considered in this study were in the submicron range, and in the simulation method, Brownian motion of particles was also taken into consideration along with electrostatic forces acting on the particles. The simulation results were compared with other investigators initial collection efficiency data, and it was found that simulation results are in good agreement with the experimental data. Based on this, we analyzed the effect of operating variables on the particle deposition morphology, which in turn affects the collection efficiency and pressure drop of the filter. In view of the simulation results on particle deposition morphology, it is clear that in the case of electret filters, particle deposition tends to take place onto the entire perimeter of fibers relatively uniformly, which may reduce the increase of pressure drop with time or extent of particle deposition compared to the conventional fibrous filter.

Size-dependent CO2 capture in chemically synthesized magnesium oxide nanocrystals

The carbon dioxide storage capacity of magnesium oxide (MgO) particles was examined as a function of particle size, shape, and surface area. Two types of MgO nanocrystals (5 nm spheres and 23 nm disks) were synthesized and compared against commercially available MgO (325 mesh/44 μm and 40 mesh/420 μm). The surface area of the four types of particles was determined by N2 gas adsorption. Carbon dioxide capture was measured at 60 °C and 600 °C using thermogravimetric analysis, with results indicating enhanced CO2 capacity correlating with increased surface area.

CoxP compounds: electrochemical conversion/partial recombination reaction and partially disproportionated nanocomposite for Li-ion battery anodes

CoxP binary compounds, CoP and Co2P, were synthesized using simple solid-state synthetic routes, and their potential as anode materials for Li-ion batteries was investigated. Electrochemical Li reactivity was possible on the CoP electrode, whereas the Co2P electrode did not react with Li. The electrochemically driven partial recombination reaction of the CoP electrode was thoroughly demonstrated using ex situ X-ray diffraction and extended X-ray absorption fine structure analyses. To enhance the electrochemical performances of CoP, its carbon-modified nanocomposite was prepared. The nanocomposite consisted of well-dispersed CoP (active with Li) and Co2P (inactive with Li) nanocrystallites, as well as amorphous P within the amorphous carbon matrix. The partially disproportionated CoP/C nanocomposite electrode exhibited good electrochemical performance with a high initial charge capacity of 531 mA h g−1 (or 855 mA h cm−3), a cycling durability of 407 mA h g−1 (or 655 mA h cm−3) over 200 cycles, a good initial coulombic efficiency of ca. 75%, and a fast rate capability (2C: 435 mA h g−1, 3C: 410 mA h g−1).