American+Association+for+the+Advancement+of+Science
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A Novel Material for Transparent and Flexible Displays
(Research team led by Professor Sang Youl Kim from the Department of Chemistry)
The next generation of flexible and transparent displays will require a high-performing and flexible polymeric material that has the optical and thermal properties of glass. The material must be transparent to visible light and have a low coefficient of thermal expansion (CTE). Unfortunately, such a polymeric material has not been available. A KAIST research team has succeeded in making a new polymeric material with an exceptionally low CTE value while retaining high transparency and excellent thermal and mechanical properties. The method developed for amorphous polymers with a controlled CTE can be applied to control the thermal expansion of organic materials as well.
Most of objects expands upon heating and shrinks by cooling, and organic polymers have a relatively large CTE compared to that of ceramics or metals. Thin, light-weight planar substrates for semiconductor devices should have a similar CTE of ceramics. Otherwise, the device can be cracked due to the stress caused by thermal expansion and contraction. Therefore, matching the CTE of the semiconductor device and the substrate is crucial for successful manufacturing of display devices. Forming a network structure by connecting polymer chains is a well-known method of reducing the CTE of amorphous polymers. However, polymers with a network structure eventually lose their flexibility and becomes brittle.
As an alternative method, Professor Sang Youl Kim from the Department of Chemistry and his team chose to adjust the distance and interaction between polymer chains. Thermal expansion and contraction of polymer films can be minimized by introducing interaction forces between the polymer chains and by arranging the direction of the force perpendicularly. The team successfully implemented this approach by appropriately designing the chemical structure of a transparent polymeric material. It is called poly (amide-imide) film, which is a transparent, flexible, and high-performing polymeric material. It is thermally stable enough to be used in the AMOLED (active-matrix organic light-emitting diode) fabrication process (stable at >400℃) with a low CTE (4ppm/℃).
The team made IGZO TFT (Indium Gallium Zinc Oxide Thin Film Transistor) devices on the newly synthesized transparent poly(amide-imide) film, and confirmed that the device could indeed operate normally even when it is folded down to a radius of 1mm.
Professor Kim said, “Our results suggest a way of controlling the thermal expansion of amorphous polymers similar to a level of glass without chemical cross-linking, which has long been regarded as a challenging problem. At the same time, we succeeded in making the polymer transparent and flexible. We expect that it can be applied to controlling the thermal expansion of various organic materials.”
This research, led by researchers Sun Dal Kim and Byungyoung Lee, was published in Science Advances on October 26. (DOI: 10.1126/sciadv.aau1956v)
2019.01.24 View 5555 -
Photonic Capsules for Injectable Laser Resonators
A KAIST research group presented photonic capsules for injectable laser resonators using microfluidic technology. The capsule’s diameter is comparable to a human hair and stable in gas and liquid media, so it is injectable into any target volume.
The research group headed by Professor Shin-Hyun Kim in the Department of Chemical and Biomolecular Engineering applied an interesting optical property from nature. Professor Kim, who has dived deep into photonic materials research inspired from nature such as the Morpho butterfly, used a trait of beetles this time.
Chrysina gloriosa, commonly known as the glorious beetle, shows a green color similar to leaves when illuminated by left-handed, circularly-polarized light while showing no color with right-handed, circularly-polarized light. This unique optical feature helps the beetles communicate with each other and protects them from predators.
The principle behind this interesting optical property of the beetles relies on helical nanostructures with left-handedness that are present on the shell of the beetles. The helical structures reflect a circularly-polarized light with the same handedness of the helix at the wavelength selected by the helical pitch through optical interference.
Such helical nanostructures can be artificially created using liquid crystals (LCs). LCs with a helical arrangement are referred to as cholesteric LCs (CLCs). The CLCs exhibit the polarization-dependent reflection of light in the same manner as the beetles and have been used for various photonic applications.
In particular, CLCs have been cast to a film format that serves as mirrorless laser resonators, unlike conventional lasing systems. However, the film-type CLCs are large in size and show unidirectional emission, which restricts the use of CLC resonators in microenvironments.
To overcome these limitations, Professor Kim’s group has encapsulated the CLCs with dual shells using microfluidic technology. The inner shell is a water layer that promotes the alignment of LC molecules and the outer shell is an elastic polymer layer that secures capsule stability and enables reversible mechanical deformation. The spherical symmetry of the capsules enables omnidirectional laser emissions. Moreover, laser intensity and lasing direction can be further controlled by deforming the capsules, while its wavelength remains tunable. This new type of CLC laser resonator is promising for laser treatments in various biomedical applications.
Professor Kim said, “The helical nanostructure used in the laser resonator resembles that of the shell of chrysina gloriosa. Humans learn from nature and engineer materials to create something unprecedented.”
This research was led by graduate student Sang Seok Lee and an article entitled “Wavelength-tunable and shape-reconfigurable photonic capsule resonators containing cholesteric liquid crystals” was published online on June 22, in Science Advances.
Figure 1. Chrysina gloriosa illuminated by left-handed (left panel) and right-handed (right panel) circularly-polarized lights.
(Image source: https://doi.org/10.1016/j.cub.2010.05.036 , permitted for reuse in news media)
Figure 2. Composition (left panel) and optical microscopy image (right panel) of the capsule-type laser resonator
2018.07.05 View 8578 -
Successful Synthesis of Gamma-Lanctam Rings from Hydrocarbons
(The team of Professor Chang, far right, at the Department of Chemistry)
KAIST chemists have designed a novel strategy to synthesize ring-shaped cyclic molecules, highly sought-after by pharmaceutical and chemical industries, and known as gamma-lactams. This study describes how these five-membered rings can be prepared from inexpensive and readily available feedstock hydrocarbons, as well as from complex organic molecules, such as amino acids and steroids.
Gamma-lactams find several applications in medicinal, synthetic, and material chemistry. For example, they are included in a large number of pharmaceutically active compounds with antibiotic, anti-inflammatory, and anti-tumoral functions. This research was published in Science on March 2.
Conversion of hydrocarbons into nitrogen-containing compounds is an important area of research, where the challenge lies in breaking strong carbon-hydrogen (C−H) bonds, and converting them into carbon-nitrogen (C–N) bonds in a controlled fashion. For this reason, hydrocarbons are difficult to use as starting materials, albeit the fact that they exist in large quantities in nature.
Over the last 35 years, chemists have found ways of converting simple hydrocarbons into nitrogen-containing rings, such as indoles or pyrrolidines, but gamma-lactams proved impossible to prepare using the same approaches. Researchers hypothesized that such failure was due to alternative chemical pathways that steer the reaction away from the wanted rings: The reaction intermediate (carbonylnitrene) quickly breaks down into unsought products. Using computer models of the desired and undesired reaction pathways, the team found a strategy to completely shut down the latter in order to obtain the longed-for gamma-lactams. For the first time, these four carbons and one nitrogen cyclic molecules were obtained directly from simple feedstock chemicals.
Led by Professor Chang Sukbok at the Department of Chemistry, the team designed the winning reaction with the help of computer simulations that analyze the reaction mechanisms and calculate the energy required for the reaction to take place. According to such computer predictions, the reaction could follow three pathways, leading to the formation of either the desired gamma-lactam, an unwanted product (isocyanate), or the degradation of the catalyst caused by the substrate reacting with the catalyst backbone. Combining experimental observations and detailed computer simulations, the team designed an iridium-based catalyst, highly selective for the gamma-lactam formation. In this way, the two undesired pathways were systematically shut down, leaving the formation of the nitrogen-containing ring as the only possible outcome. Professor Chang is also in charge of the Center for Catalytic Hydrocarbon Functionalizations at the Institute for Basic Science (IBS).
“With this work we offer a brand new solution to a long-standing challenge and demonstrate the power of what we call mechanism-based reaction development,” explains Professor Baik Mu-Hyun, a corresponding author of the study.
Beyond using cheap feedstock hydrocarbons as substrates, the team was also successful in converting amino acids, steroids, and other bio-relevant molecules into gamma-lactams, which might find a variety of applications as plant insecticide, drugs against parasitic worms, or anti-aging agents. This new synthetic technology gives much easier access to these complicated molecules and will enable the development of potential drugs in a much shorter amount of time at a lower cost.
Figure 1: Selective amidation reaction using newly designed iridium (Ir) catalysts. Abundant in nature Hydrocarbons are used as substrates to synthesize nitrogen-containing ring, called gamma-lactams.
Figure 2: Three possible reaction pathways and energy barriers predicted by computational chemistry. The scientists developed new iridium-based catalysts that are highly selective for the C–H insertion pathway which leads to the desired gamma-lactam molecules.
Figure 3: Interesting gamma-lactams derived from natural and unnatural amino acids, steroids, etc., which may be used to protect plants against insects, fight parasitic worms, or as anti-aging agents.
2018.03.02 View 7785 -
Structural Insight into the Molecular Mechanism of PET Degradation
A KAIST metabolic engineering research team has newly suggested a molecular mechanism showing superior degradability of poly ethylene terephthalate (PET).
This is the first report to simultaneously determine the 3D crystal structure of Ideonella sakaiensis PETase and develop the new variant with enhanced PET degradation.
Recently, diverse research projects are working to address the non-degradability of materials. A poly ethylene terephthalate (PET)-degrading bacterium called Ideonella sakaiensis was recently identified for the possible degradation and recycling of PET by Japanese team in Science journal (Yoshida et al., 2016). However, the detailed molecular mechanism of PET degradation has not been yet identified.
The team under Distinguished Professor Sang Yup Lee of the Department of Chemical and Biomolecular Engineering and the team under Professor Kyung-Jin Kim of the Department of Biotechnology at Kyungpook National University conducted this research. The findings were published in Nature Communications on January 26.
This research predicts a special molecular mechanism based on the docking simulation between PETase and a PET alternative mimic substrate. Furthermore, they succeeded in constructing the variant for IsPETase with enhanced PET-degrading activity using structural-based protein engineering.
It is expected that the new approaches taken in this research can be background for further study of other enzymes capable of degrading not only PET but other plastics as well.
PET is very important source in our daily lives. However, PET after use causes tremendous contamination issues to our environment due to its non-biodegradability, which has been a major advantage of PET. Conventionally, PET is disposed of in landfills, using incineration, and sometimes recycling using chemical methods, which induces additional environmental pollution. Therefore, a new development for highly-efficient PET degrading enzymes is essential to degrade PET using bio-based eco-friendly methods.
Recently, a new bacterial species, Ideonella sakaiensis, which can use PET as a carbon source, was isolated. The PETase of I. sakaiensis (IsPETase) can degrade PET with relatively higher success than other PET-degrading enzymes. However, the detailed enzyme mechanism has not been elucidated, hindering further studies.
The research teams investigated how the substrate binds to the enzyme and which differences in enzyme structure result in significantly higher PET degrading activity compared with other cutinases and esterases, which make IsPETase highly attractive for industrial applications toward PET waste recycling.
Based on the 3D structure and related biochemical studies, they successfully predicted the reasons for extraordinary PET degrading activity of IsPETase and suggested other enzymes that can degrade PET with a newly-classified phylogenetic tree. The team proposed that 4 MHET moieties are the most properly matched substrates due to a cleft on structure even with the 10-20-mers for PET. This is meaningful in that it is the first docking simulation between PETase and PET, not its monomer.
Furthermore, they succeeded in developing a new variant with much higher PET-degrading activity using a crystal structure of this variant to show that the changed structure is better to accommodate PET substrates than wild type PETase, which will lead to developing further superior enzymes and constructing platforms for microbial plastic recycling.
Professor Lee said, “Environmental pollution from plastics remains one of the greatest challenges worldwide with the increasing consumption of plastics. We successfully constructed a new superior PET-degrading variant with the determination of a crystal structure of PETase and its degrading molecular mechanism. This novel technology will help further studies to engineer more superior enzymes with high efficiency in degrading. This will be the subject of our team’s ongoing research projects to address the global environmental pollution problem for next generation.”
This work was supported by the Technology Development Program to Solve Climate Changes on Systems Metabolic Engineering for Biorefineries (NRF-2012M1A2A2026556 and NRF-2012M1A2A2026557) from the Ministry of Science and ICT through the National Research Foundation of Korea. Further Contact: Dr. Sang Yup Lee, Distinguished Professor, KAIST, Daejeon, Korea (leesy@kaist.ac.kr, +82-42-350-3930)
(Figure: Structural insight into the molecular mechanism of poly(ethylene terephthalate) degradation and the phylogenetic tree of possible PET degrading enzymes. This schematic diagram shows the overall conceptualization for structural insight into the molecular mechanism of poly (ethylene terephthalate) degradation and the phylogenetic tree of possible PET degrading enzymes.)
2018.01.31 View 8386 -
Study Identifies the Novel Molecular Signal for Triggering Septic Shock
Professor Seyun Kim’s team at the Department of Biological Sciences reported the mechanism by which cellular signaling transduction networks are precisely controlled in mediating innate immune responses, such as sepsis, by the enzyme IPMK (Inositol polyphosphate multikinase) which is essential for inositol biosynthesis metabolism.
In collaboration with Professor Hyun Seong Roh at Seoul National University, the study’s first author, Eunha Kim, a Ph.D. candidate in Department of Biological Sciences, performed a series of cellular, biochemical, and physiological experiments searching for the new function of IPMK enzymes in macrophages. The research findings were published in Science Advances on April 21.
Professor Kim’s team has been investigating various inositol metabolites and their biosynthesis metabolism for several years and has multilaterally identified the signaling actions of IPMK for controlling cellular growth and energy homeostasis.
This research showed that the specific deletion of IPMK enzymes in macrophages could significantly reduce levels of inflammation and increase survival rates in mice when they were challenged by microbial septic shock and endotoxins. This suggests a role for IPMK enzymes in mediating innate inflammatory responses that are directly related to a host’s defense against pathogenic bacterial infection.
The team further discovered that IPMK enzymes directly bind to TRAF6 proteins, a key player in immune signaling, thus protecting TRAF6 proteins from ubiquitination reactions that are involved in protein degradation. In addition, Kim and his colleagues successfully verified this IPMK-dependent immune control by employing short peptides which can specifically interfere with the binding between IPMK enzymes and TRAF6 proteins in macrophage cells.
This research revealed a novel function of IPMK enzymes in the fine tuning of innate immune signaling networks, suggesting a new direction for developing therapeutics targeting serious medical conditions such as neuroinflammation, type 2 diabetes, as well as polymicrobial sepsis that are developed from uncontrolled host immune responses. This research was funded by the Ministry of Science, ICT and Future Planning.
(Figure: Deletion of IPMK (inositol polyphosphate multikinase) in macrophages reduces the stability of TRAF6 protein which is the key to innate immune signaling, thereby blocking excessive inflammation in response to pathological bacterial infection.)
2017.05.11 View 8218 -
Expanding the Genetic Code of Mus Musculus
Professor Hee-Sung Park of the Department of Chemistry, who garnered attention for his novel strategy of installing authentic post-translational modifications into recombinant proteins, expanded his research portfolio to another level. Professor Park’s team was the first to report the generation of a mouse strain with an expanded genetic code, allowing site-specific incorporation of unnatural amino acids.
Professor Park published the research on the new chemical biology method for achieving selective chemical modifications in proteins in Science last September. The research team, this time in collaboration with Professor Chan Bae Park of the Department of Physiology at the Ajou University School of Medicine, demonstrated temporal and spatial control of protein acetylation in various organs of the transgenic mouse using a recombinant green fluorescent protein as a model protein. This research was published in the online edition of Nature Communications on February 21.
This approach enables the rapid onset of position-specific acetylation of a target protein at any developmental stage, facilitating temporal and spatial control of protein acetylation in various organs of the transgenic mouse. Such temporal and spatial control of protein acetylation will be of prime importance for investigating many essential biological processes and human diseases at the tissue and organism level.
Almost all human proteins, the products of about 25,000 genes, are known to undergo various post-translational modifications during and after synthesis. Post-translation modifications regulate the function of cellular proteins, playing a key role in many essential processes such as delivering signals and body growth. However, the unusual protein modifications, aroused from genetic and/or environmental factors, trigger severe diseases including cancer, dementia, and diabetes.
The team inserted transgenes into the mouse genome to allocate the site-specific addition of unnatural amino acids. The researchers inserted a modified version of lysine into the house mice, which allowed for the control of the acetylation. They used recombinant green fluorescent proteins from transgenic house mice as models for control of the acetylation.
The team was also able to regulate the acetylation of specific temporal and spatial frames in the mice, restraining the abnormality in proteins to certain organs such as the liver and kidneys. The research team said the strategy will provide a powerful tool for systematic in vivo study of cellular proteins in the most commonly used mammalian model organisms for human physiology and disease. Professor Park said, “This method can be easily extended to generate a wide range of custom-made transgenic mouse strains for further investigating diverse proteins of interest.” He added, “This method can be further extended to generate a wide range of custom-made transgenic mouse strains, opening a new paradigm for investigating anti-cancer and cerebral disease treatments.
This work was supported by grants from KAIST Systems Healthcare and the Medicinal Bioconvergence Research Center and the Intelligent Synthetic Biology Center of the Global Frontier Project funded by the Ministry of Science, ICT & Future Planning and the Ministry of Food and Drug Safety.
(Figure:Temporal and spatial control of in vivo protein acetylation)
(a) Temporal expression of acetylated GFPuv in the AcK-GFPamber mouse. The expression of GFPuv in skeletal muscle, liver, and lung tissues was detected only in the AcK-injected mouse. Scale bar, 200 µm. (b) Western blotting of anti-FLAG-immunoprecipitated proteins from tissues of the AcK-GFPamber mouse. Acetylated GFPuv was produced after AcK injection. (c) Spatial expression of acetylated GFPuv in the AcK-GFPamber mouse. Acetylated GFPuv was observed only in skeletal muscle when AcK was directly delivered to the tissues. Sacle bar, 200 µm.
2017.03.27 View 8481