Seongbeom Kim

High-yield synthesis of single-crystal silicon nanoparticles as anode materials of lithium ion batteries via photosensitizer-assisted laser pyrolysis

Single crystal silicon nanoparticles (Si-NPs) of 20 nm were produced via laser pyrolysis with a virtually complete conversion from SiH4 to Si-NPs. SF6 was used as the photosensitizer to transfer laser beam energy to silicon precursors, dramatically enhancing crystallinity of Si-NPs and their production efficiency. By using their well-developed crystalline structure, the directional volume expansion of Si-NPs was confirmed during lithiation. Lithiation/delithiation kinetics of our Si-NPs was superior to that of their amorphous counterparts due to the footprinted Li+ pathways formed during amorphization.

Enhanced Performance of a Polymer Solar Cell upon Addition of Free-Standing, Freshly Etched, Photoluminescent Silicon Nanocrystals

We demonstrate an organic–inorganic hybrid solar cell using poly(3-hexylthiophene) (P3HT)/[6,6]-phenyl-C61-butyric acid methyl ester (PCBM) and silicon nanocrystals (Si-NCs). To achieve an enhanced response in the hybrid layer, Si-NCs were freshly etched and blended with P3HT/PCBM. The incorporation of Si-NCs into the bulk heterojunction structure induced the coupling of optical excitation between the polymers and Si-NCs and led to an extended optical excitation response. A hybrid solar cell exhibited a 26% increase in JSC relative to an identical cell prepared without the Si-NCs. Consequently, improved power conversion efficiency is obtained by the addition of Si-NCs into polymers.

Capacity retention behavior and morphology evolution of SixGe1−x nanoparticles as lithium-ion battery anode

Engineering silicon into nanostructures has been a well-adopted strategy to improve the cyclic performance of silicon as a lithium-ion battery anode. Here, we show that the electrode performance can be further improved by alloying silicon with germanium. We have evaluated the electrode performance of SixGe1-x nanoparticles (NPs) with different compositions. Experimentally, SixGe1-x NPs with compositions approaching Si50Ge50 are found to have better cyclic retention than both Si-rich and Ge-rich NPs. During the charge/discharge process, NP merging and Si-Ge homogenization are observed. In addition, a distinct morphology difference is observed after 100 cycles, which is believed to be responsible for the different capacity retention behavior. The present study on SixGe1-x alloy NPs sheds light on the development of Si-based electrode materials for stable operation in lithium-ion batteries (e.g., through a comprehensive design of material structure and chemical composition). The investigation of composition-dependent morphology evolution in the delithiated Li-SiGe ternary alloy also significantly broadens our understanding of dealloying in complex systems, and it is complementary to the well-established understanding of dealloying behavior in binary systems (e.g., Au-Ag alloys).

ZnO decorated germanium nanoparticles as anode materials in Li-ion batteries

Germanium exhibits high charge capacity and high lithium diffusivity, both are the key requirements for electrode materials in high performance lithium ion batteries (LIBs). However, high volume expansion and segregation from the electrode during charge-discharge cycling have limited use of germanium in LIBs. Here, we demonstrate that ZnO decorated Ge nanoparticles (Ge@ZnO NPs) can overcome these limitations of Ge as an LIB anode material. We produced Ge NPs at high rates by laser pyrolysis of GeH4, then coated them with solution phase synthesized ZnO NPs. Half-cell tests revealed dramatically enhanced cycling stability and higher rate capability of Ge@ZnO NPs compared to Ge NPs. Enhancements arise from the core-shell structure of Ge@ZnO NPs as well as production of metallic Zn from the ZnO layer. These findings not only demonstrate a new surface treatment for Ge NPs, but also provide a new opportunity for development of high-rate LIBs.

Production of pristine, sulfur-coated and silicon-alloyed germanium nanoparticles via laser pyrolysis

Here we demonstrate production of three types of germanium containing nanoparticles (NPs) by laser pyrolysis of GeH4 and characterize their sizes, structures and composition. Pristine Ge NPs were fabricated with 50 standard cubic centimeter per minute (sccm) of GeH4 and 25 sccm of SF6 as a photosensitizer gas, while sulfur-coated Ge NPs were produced with 25 sccm of GeH4 and 50 sccm of SF6. The laser pyrolysis of SiH4/GeH4 mixtures produced Si1-xGex alloy NPs. Effects of key process parameters including laser intensity and gas flow rates on NP properties have been investigated. The ability of the laser pyrolysis technique to flexibly produce a variety of germanium-containing NPs, as illustrated in this study shows promise for commercial-scale production of new nanomaterials as high purity dry powders.