Hye Ryoung Lee

Hierarchical nanostructured conducting polymer hydrogel with high electrochemical activity

Conducting polymer hydrogels represent a unique class of materials that synergizes the advantageous features of hydrogels and organic conductors and have been used in many applications such as bioelectronics and energy storage devices. They are often synthesized by polymerizing conductive polymer monomer within a nonconducting hydrogel matrix, resulting in deterioration of their electrical properties. Here, we report a scalable and versatile synthesis of multifunctional polyaniline (PAni) hydrogel with excellent electronic conductivity and electrochemical properties. With high surface area and three-dimensional porous nanostructures, the PAni hydrogels demonstrated potential as high-performance supercapacitor electrodes with high specific capacitance (∼480 F·g-1), unprecedented rate capability, and cycling stability (∼83% capacitance retention after 10,000 cycles). The PAni hydrogels can also function as the active component of glucose oxidase sensors with fast response time (∼0.3 s) and superior sensitivity (∼16.7 μA·mM-1). The scalable synthesis and excellent electrode performance of the PAni hydrogel make it an attractive candidate for bioelectronics and future-generation energy storage electrodes.

First-row transition metal dichalcogenide catalysts for hydrogen evolution reaction

A group of first-row transition metal dichalcogenides (ME2, M = Fe, Co, Ni; E = S, Se) are introduced as non-precious HER catalysts in an acidic electrolyte. They exhibit excellent catalytic activity especially in their nanoparticle form. These compounds expand and enrich the family of high performance HER catalysts.

Performance enhancement of metal nanowire transparent conducting electrodes by mesoscale metal wires.

For transparent conducting electrodes in optoelectronic devices, electrical sheet resistance and optical transmittance are two of the main criteria. Recently, metal nanowires have been demonstrated to be a promising type of transparent conducting electrode because of low sheet resistance and high transmittance. Here we incorporate a mesoscale metal wire (1-5 μm in diameter) into metal nanowire transparent conducting electrodes and demonstrate at least a one order of magnitude reduction in sheet resistance at a given transmittance. We realize experimentally a hybrid of mesoscale and nanoscale metal nanowires with high performance, including a sheet resistance of 0.36 Ω sq(-1) and transmittance of 92%. In addition, the mesoscale metal wires are applied to a wide range of transparent conducting electrodes including conducting polymers and oxides with improvement up to several orders of magnitude. The metal mesowires can be synthesized by electrospinning methods and their general applicability opens up opportunities for many transparent conducting electrode applications.

A high tap density secondary silicon particle anode fabricated by scalable mechanical pressing for lithium-ion batteries

Much progress has been made in developing high capacity lithium ion battery electrode materials such as silicon anodes. With the powerful nanomaterial design approach, cycle life of silicon anodes has been increased significantly. However, nanomaterials have three major issues to be addressed, including severe side reactions due to a large surface area, low tap density and poor scalability. Nanostructured Si secondary clusters (nano-Si SC) are promising for reducing side reactions and increasing tap density, yet the scalability and tap density could still be further improved. Here, we propose a mechanical approach for SC fabrication to address all the problems. With the mechanical approach, >20 g of nano-Si SC per batch was produced even at our university lab scale, with >95% yield. Moreover, much denser packing of nanostructures can be achieved (1.38 g cm−3, pellet form), which gives much higher tap density (0.91 g cm−3, powder form) and better electrical contact. Accordingly, over 95% of initial capacity is retained after 1400 cycles at 1C, with an average specific capacity of ∼1250 mA h g−1. Stable cycling with >2 mg cm−2 of areal mass loading (∼3.5 mA h cm−2) is obtained. After uniformly integrating carbon nanotubes (CNTs) into SCs, intracluster electrical conductivity is further improved. As a result, notably enhanced rate capability is attained, with a high reversible specific capacity of ∼1140 mA h g−1 and ∼880 mA h g−1 at 2C and 4C, respectively.

High Ionic Conductivity of Composite Solid Polymer Electrolyte via In Situ Synthesis of Monodispersed SiO2 Nanospheres in Poly(ethylene oxide)

High ionic conductivity solid polymer electrolyte (SPE) has long been desired for the next generation high energy and safe rechargeable lithium batteries. Among all of the SPEs, composite polymer electrolyte (CPE) with ceramic fillers has garnered great interest due to the enhancement of ionic conductivity. However, the high degree of polymer crystallinity, agglomeration of ceramic fillers, and weak polymer-ceramic interaction limit the further improvement of ionic conductivity. Different from the existing methods of blending preformed ceramic particles with polymers, here we introduce an in situ synthesis of ceramic filler particles in polymer electrolyte. Much stronger chemical/mechanical interactions between monodispersed 12 nm diameter SiO2 nanospheres and poly(ethylene oxide) (PEO) chains were produced by in situ hydrolysis, which significantly suppresses the crystallization of PEO and thus facilitates polymer segmental motion for ionic conduction. In addition, an improved degree of LiClO4 dissociation can also be achieved. All of these lead to good ionic conductivity (1.2 × 10(-3) S cm(-1) at 60 °C, 4.4 × 10(-5) S cm(-1) at 30 °C). At the same time, largely extended electrochemical stability window up to 5.5 V can be observed. We further demonstrated all-solid-state lithium batteries showing excellent rate capability as well as good cycling performance.

Tuning the threshold voltage of carbon nanotube transistors by n-type molecular doping for robust and flexible complementary circuits

Significance Highly noise-resistant logic gates are needed for large-scale circuits. This was challenging previously with carbon nanotube circuits due to the lack of control of the threshold voltages of nanotube transistors. We demonstrate the use of dopants to tune the charge carrier density of carbon nanotubes films and hence precisely control the threshold voltages of carbon nanotube transistors. This doping method is highly versatile and can be applied through inkjet printing. With this technique, we demonstrate highly noise-resistant and low power consumption carbon nanotube logic gates on a flexible substrate. This work places carbon nanotubes in a highly competitive position for large-scale solution-processed flexible circuits. Tuning the threshold voltage of a transistor is crucial for realizing robust digital circuits. For silicon transistors, the threshold voltage can be accurately controlled by doping. However, it remains challenging to tune the threshold voltage of single-wall nanotube (SWNT) thin-film transistors. Here, we report a facile method to controllably n-dope SWNTs using 1H-benzoimidazole derivatives processed via either solution coating or vacuum deposition. The threshold voltages of our polythiophene-sorted SWNT thin-film transistors can be tuned accurately and continuously over a wide range. Photoelectron spectroscopy measurements confirmed that the SWNT Fermi level shifted to the conduction band edge with increasing doping concentration. Using this doping approach, we proceeded to fabricate SWNT complementary inverters by inkjet printing of the dopants. We observed an unprecedented noise margin of 28 V at VDD = 80 V (70% of 1/2VDD) and a gain of 85. Additionally, robust SWNT complementary metal−oxide−semiconductor inverter (noise margin 72% of 1/2VDD) and logic gates with rail-to-rail output voltage swing and subnanowatt power consumption were fabricated onto a highly flexible substrate.

Vertical Heterostructure of Two-Dimensional MoS2 and WSe2 with Vertically Aligned Layers

Two-dimensional (2D) layered materials consist of covalently bonded 2D atomic layers stacked by van der Waals interactions. Such anisotropic bonding nature gives rise to the orientation-dependent functionalities of the 2D layered materials. Different from most studies of 2D materials with their atomic layers parallel to substrate, we have recently developed layer vertically aligned 2D material nanofilms. Built on these developments, here, we demonstrate the synthesis of vertical heterostructure of n-type MoS2 and p-type WSe2 with vertically aligned atomic layers. Thin film of MoS2/WSe2 vertical structure was successfully synthesized without significant alloy formation. The heterostructure synthesis is scalable to a large area over 1 cm(2). We demonstrated the pn junction diode behavior of the heterostructure device. This novel device geometry opens up exciting opportunities for a variety of electronic and optoelectronic devices, complementary to the recent interesting vertical heterostructures with horizontal atomic layers.

Tuning the Dirac point in CVD-grown graphene through solution processed n-type doping with 2-(2-methoxyphenyl)-1,3-dimethyl-2,3-dihydro-1H-benzoimidazole.

Controlling the Dirac point of graphene is essential for complementary circuits. Here, we describe the use of 2-(2-methoxyphenyl)-1,3-dimethyl-2,3-dihydro-1H-benzoimidazole (o-MeO-DMBI) as a strong n-type dopant for chemical-vapor-deposition (CVD) grown graphene. The Dirac point of graphene can be tuned significantly by spin-coating o-MeO-DMBI solutions on the graphene sheets at different concentrations. The transport of graphene can be changed from p-type to ambipolar and finally n-type. The electron transfer between o-MeO-DMBI and graphene was additionally confirmed by Raman imaging and photoemission spectroscopy (PES) measurements. Finally, we fabricated a complementary inverter via inkjet printing patterning of o-MeO-DMBI solutions on graphene to demonstrate the potential of o-MeO-DMBI n-type doping on graphene for future applications in electrical devices.

3D Porous Sponge-Inspired Electrode for Stretchable Lithium-Ion Batteries

A stretchable Li4 Ti5 O12 anode and a LiFePO4 cathode with 80% stretchability are prepared using a 3D interconnected porous polydimethylsiloxane sponge based on sugar cubes. 82% and 91% capacity retention for anode and cathode are achieved after 500 stretch-release cycles. Slight capacity decay of 6% in the battery using the electrode in stretched state is observed.

Nanofiber Air Filters with High-Temperature Stability for Efficient PM2.5 Removal from the Pollution Sources

Here, we developed high-efficiency (>99.5%) polyimide-nanofiber air filters for the high temperature PM2.5 removal. The polyimide nanofibers exhibited high thermal stability, and the PM2.5 removal efficiency was kept unchanged when temperature ranged from 25-370 °C. These filters had high air flux with very low pressure drop. They could continuously work for >120 h for PM2.5 index >300. A field-test showed that they could effectively remove >99.5% PM particles from car exhaust at high temperature.