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New Nanoparticle Drug Combination For Atherosclerosis
Physicochemical cargo-switching nanoparticles (CSNP) designed by KAIST can help significantly reduce cholesterol and macrophage foam cells in arteries, which are the two main triggers for atherosclerotic plaque and inflammation. The CSNP-based combination drug delivery therapy was proved to exert cholesterol-lowering, anti-inflammatory, and anti-proliferative functions of two common medications for treating and preventing atherosclerosis that are cyclodextrin and statin. Professor Ji-Ho Park and Dr. Heegon Kim from KAIST’s Department of Bio and Brain Engineering said their study has shown great potential for future applications with reduced side effects. Atherosclerosis is a chronic inflammatory vascular disease that is characterized by the accumulation of cholesterol and cholesterol-loaded macrophage foam cells in the intima. When this atherosclerotic plaque clogs and narrows the artery walls, they restrict blood flow and cause various cardiovascular conditions such as heart attacks and strokes. Heart attacks and strokes are the world’s first and fifth causes of death respectively. Oral statin administration has been used in clinics as a standard care for atherosclerosis, which is prescribed to lower blood cholesterol and inhibit its accumulation within the plaque. Although statins can effectively prevent the progression of plaque growth, they have only shown modest efficacy in eliminating the already-established plaque. Therefore, patients are required to take statin drugs for the rest of their lives and will always carry the risk of plaque ruptures that can trigger a blood clot. To address these issues, Professor Park and Dr. Kim exploited another antiatherogenic agent called cyclodextrin. In their paper published in the Journal of Controlled Release on March 10, Professor Park and Dr. Kim reported that the polymeric formulation of cyclodextrin with a diameter of approximately 10 nanometers(nm) can accumulate within the atherosclerotic plaque 14 times more and effectively reduce the plaque even at lower doses, compared to cyclodextrin in a non-polymer structure. Moreover, although cyclodextrin is known to have a cytotoxic effect on hair cells in the cochlea, which can lead to hearing loss, cyclodextrin polymers developed by Professor Park’s research group exhibited a varying biodistribution profile and did not have this side effect. In the follow-up study reported in ACS Nano on April 28, the researchers exploited both cyclodextrin and statin and form the cyclodextrin-statin self-assembly drug complex, based on previous findings that each drug can exert local anti-atherosclerosis effect within the plaque. The complex formation processes were optimized to obtain homogeneous and stable nanoparticles with a diameter of about 100 nm for systematic injection. The therapeutic synergy of cyclodextrin and statin could reportedly enhance plaque-targeted drug delivery and anti-inflammation. Cyclodextrin led to the regression of cholesterol in the established plaque, and the statins were shown to inhibit the proliferation of macrophage foam cells. The study suggested that combination therapy is required to resolve the complex inflammatory cholesterol-rich microenvironment within the plaque. Professor Park said, “While nanomedicine has been mainly developed for the treatment of cancers, our studies show that nanomedicine can also play a significant role in treating and preventing atherosclerosis, which causes various cardiovascular diseases that are the leading causes of death worldwide.” This work was supported by KAIST and the National Research Foundation (NRF) of Korea. Publications: 1. Heegon Kim, Junhee Han, and Ji-Ho Park. (2020) ‘Cyclodextrin polymer improves atherosclerosis therapy and reduces ototoxicity’ Journal of Controlled Release. Volume 319. Page 77-86. Available online at https://doi.org/10.1016/j.jconrel.2019.12.021 2. Kim, H., et al. (2020) ‘Affinity-Driven Design of Cargo-Switching Nanoparticles to Leverage a Cholesterol-Rich Microenvironment for Atherosclerosis Therapy’ ACS Nano. Available online at https://doi.org/10.1021/acsnano.9b08216 Profile: Ji-Ho Park, Ph.D. Associate Professor email@example.com http://openwetware.org/wiki/Park_Lab Biomaterials Engineering Laboratory (BEL) Department of Bio and Brain Engineering (BIOENG) Korea Advanced Institute of Science and Technology (KAIST) https://www.kaist.ac.kr Daejeon 34141, Korea Profile: Heegon Kim, Ph.D. Postdoctoral Researcher firstname.lastname@example.org BEL, BIOENG, KAIST (END)
Simple Molecular Reagents to Treat Alzheimer’s Disease
- Researchers report minimalistic principles for designing small molecules with multiple reactivities against dementia. - Sometimes the most complex problems actually have very simple solutions. A group of South Korean researchers reported an efficient and effective redox-based strategy for incorporating multiple functions into simple molecular reagents against neurodegenerative disorders. The team developed redox-active aromatic molecular reagents with a simple structural composition that can simultaneously target and modulate various pathogenic factors in complex neurodegenerative disorders such as Alzheimer’s disease. Alzheimer’s disease is one of the most prevalent neurodegenerative disorders, affecting one in ten people over the age of 65. Early-onset dementia also increasingly affects younger people. A number of pathogenic elements such as reactive oxygen species, amyloid-beta, and metal ions have been suggested as potential causes of Alzheimer’s disease. Each element itself can lead to Alzheimer’s disease, but interactions between them may also aggravate the patient’s condition or interfere with the appropriate clinical care. For example, when interacting with amyloid-beta, metal ions foster the aggregation and accumulation of amyloid-beta peptides that can induce oxidative stress and toxicity in the brain and lead to neurodegeneration. Because these pathogenic factors of Alzheimer’s disease are intertwined, developing therapeutic agents that are capable of simultaneously regulating metal ion dyshomeostasis, amyloid-beta agglutination, and oxidative stress responses remains a key to halting the progression of the disease. A research team led by Professor Mi Hee Lim from the Department of Chemistry at KAIST demonstrated the feasibility of structure-mechanism-based molecular design for controlling a molecule’s chemical reactivity toward the various pathological factors of Alzheimer’s disease by tuning the redox properties of the molecule. This study, featured as the ‘ACS Editors’ Choice’ in the May 6th issue of the Journal of the American Chemical Society (JACS), was conducted in conjunction with KAIST Professor Mu-Hyun Baik’s group and Professor Joo-Young Lee’s group at the Asan Medical Center. Professor Lim and her collaborators rationally designed and generated 10 compact aromatic molecules presenting a range of redox potentials by adjusting the electronic distribution of the phenyl, phenylene, or pyridyl moiety to impart redox-dependent reactivities against the multiple pathogenic factors in Alzheimer’s disease. During the team’s biochemical and biophysical studies, these designed molecular reagents displayed redox-dependent reactivities against numerous desirable targets that are associated with Alzheimer’s disease such as free radicals, metal-free amyloid-beta, and metal-bound amyloid-beta. Further mechanistic results revealed that the redox properties of these designed molecular reagents were essential for their function. The team demonstrated that these reagents engaged in oxidative reactions with metal-free and metal-bound amyloid-beta and led to chemical modifications. The products of such oxidative transformations were observed to form covalent adducts with amyloid-beta and alter its aggregation. Moreover, the administration of the most promising candidate molecule significantly attenuated the amyloid pathology in the brains of Alzheimer’s disease transgenic mice and improved their cognitive defects. Professor Lim said, “This strategy is straightforward, time-saving, and cost-effective, and its effect is significant. We are excited to help enable the advancement of new therapeutic agents for neurodegenerative disorders, which can improve the lives of so many patients.” This work was supported by the National Research Foundation (NRF) of Korea, the Institute for Basic Science (IBS), and the Asan Institute for Life Sciences. Image credit: Professor Mi Hee Lim, KAIST Image usage restrictions: News organizations may use or redistribute this image, with proper attribution, as part of the news coverage of this paper only. Publication: Kim, M. et al. (2020) ‘Minimalistic Principles for Designing Small Molecules with Multiple Reactivities against Pathological Factors in Dementia.’ Journal of the American Chemical Society (JACS), Volume 142, Issue 18, pp.8183-8193. Available online at https://doi.org/10.1021/jacs.9b13100 Profile: Mi Hee Lim Professor email@example.com http://sites.google.com/site/miheelimlab Lim Laboratory Department of Chemistry KAIST Profile: Mu-Hyun Baik Professor firstname.lastname@example.org https://baik-laboratory.com/ Baik Laboratory Department of Chemistry KAIST Profile: Joo-Yong Lee Professor email@example.com Asan Institute for Life Sciences Asan Medical Center (END)
Wearable Strain Sensor Using Light Transmittance Helps Measure Physical Signals Better
KAIST researchers have developed a novel wearable strain sensor based on the modulation of optical transmittance of a carbon nanotube (CNT)-embedded elastomer. The sensor is capable of sensitive, stable, and continuous measurement of physical signals. This technology, featured in the March 4th issue of ACS Applied Materials & Interfaces as a front cover article, shows great potential for the detection of subtle human motions and the real-time monitoring of body postures for healthcare applications. A wearable strain sensor must have high sensitivity, flexibility, and stretchability, as well as low cost. Those used especially for health monitoring should also be tied to long-term solid performance, and be environmentally stable. Various stretchable strain sensors based on piezo-resistive and capacitive principles have been developed to meet all these requirements. Conventional piezo-resistive strain sensors using functional nanomaterials, including CNTs as the most common example, have shown high sensitivity and great sensing performance. However, they suffer from poor long-term stability and linearity, as well as considerable signal hysteresis. As an alternative, piezo-capacitive strain sensors with better stability, lower hysteresis, and higher stretchability have been suggested. But due to the fact that piezo-capacitive strain sensors exhibit limited sensitivity and strong electromagnetic interference caused by the conductive objects in the surrounding environment, these conventional stretchable strain sensors are still facing limitations that are yet to be resolved. A KAIST research team led by Professor Inkyu Park from the Department of Mechanical Engineering suggested that an optical-type stretchable strain sensor can be a good alternative to resolve the limitations of conventional piezo-resistive and piezo-capacitive strain sensors, because they have high stability and are less affected by environmental disturbances. The team then introduced an optical wearable strain sensor based on the light transmittance changes of a CNT-embedded elastomer, which further addresses the low sensitivity problem of conventional optical stretchable strain sensors. In order to achieve a large dynamic range for the sensor, Professor Park and his researchers chose Ecoflex as an elastomeric substrate with good mechanical durability, flexibility, and attachability on human skin, and the new optical wearable strain sensor developed by the research group actually shows a wide dynamic range of 0 to 400%. In addition, the researchers propagated the microcracks under tensile strain within the film of multi-walled CNTs embedded in the Ecoflex substrate, changing the optical transmittance of the film. By doing so, it was possible for them to develop a wearable strain sensor having a sensitivity 10 times higher than conventional optical stretchable strain sensors. The proposed sensor has also passed the durability test with excellent results. The sensor’s response after 13,000 sets of cyclic loading was stable without any noticeable drift. This suggests that the sensor response can be used without degradation, even if the sensor is repeatedly used for a long time and in various environmental conditions. Using the developed sensor, the research team could measure the finger bending motion and used it for robot control. They also developed a three-axes sensor array for body posture monitoring. The sensor was able to monitor human motions with small strains such as a pulse near the carotid artery and muscle movement around the mouth during pronunciation. Professor Park said, “In this study, our group developed a new wearable strain sensor platform that overcomes many limitations of previously developed resistive, capacitive, and optical-type stretchable strain sensors. Our sensor could be widely used in a variety of fields including soft robotics, wearable electronics, electronic skin, healthcare, and even entertainment.” This work was supported by the National Research Foundation (NRF) of Korea. Publication: Jimin Gu, Donguk Kwon, Junseong Ahn, and Inkyu Park. (2020) “Wearable Strain sensors Using Light Transmittance Change of Carbon Nanotube-Embedded Elastomers with Microcracks” ACS Applied Materials & Interfaces. Volume 12. Issue 9. Available online at https://doi.org/10.1021/acsami.9b18069 Profile: Inkyu Park Professor firstname.lastname@example.org http://mintlab1.kaist.ac.kr Micro/Nano Transducers Laboratory (MINT Lab) Department of Mechanical Engineering (ME)Korea Advanced Institute of Science and Technology (KAIST) Profile: Jimin Gu Ph.D. Candidate email@example.com http://mintlab1.kaist.ac.kr MINT Lab KAIST ME (END)
New Graphene-Based Metasurface Capable of Independent Amplitude and Phase Control of Light
Researchers described a new strategy of designing metamolecules that incorporates two independently controllable subwavelength meta-atoms. This two-parametric control of the metamolecule secures the complete control of both amplitude and the phase of light. A KAIST research team in collaboration with the University of Wisconsin-Madison theoretically suggested a graphene-based active metasurface capable of independent amplitude and phase control of mid-infrared light. This research gives a new insight into modulating the mid-infrared wavefront with high resolution by solving the problem of the independent control of light amplitude and phase, which has remained a long-standing challenge. Light modulation technology is essential for developing future optical devices such as holography, high-resolution imaging, and optical communication systems. Liquid crystals and a microelectromechanical system (MEMS) have previously been utilized to modulate light. However, both methods suffer from significantly limited driving speeds and unit pixel sizes larger than the diffraction limit, which consequently prevent their integration into photonic systems. The metasurface platform is considered a strong candidate for the next generation of light modulation technology. Metasurfaces have optical properties that natural materials cannot have, and can overcome the limitations of conventional optical systems, such as forming a high-resolution image beyond the diffraction limit. In particular, the active metasurface is regarded as a technology with a wide range of applications due to its tunable optical characteristics with an electrical signal. However, the previous active metasurfaces suffered from the inevitable correlation between light amplitude control and phase control. This problem is caused by the modulation mechanism of conventional metasurfaces. Conventional metasurfaces have been designed such that a metaatom only has one resonance condition, but a single resonant design inherently lacks the degrees of freedom to independently control the amplitude and phase of light. The research team made a metaunit by combining two independently controllable metaatoms, dramatically improving the modulation range of active metasurfaces. The proposed metasurface can control the amplitude and phase of the mid-infrared light independently with a resolution beyond the diffraction limit, thus allowing complete control of the optical wavefront. The research team theoretically confirmed the performance of the proposed active metasurface and the possibility of wavefront shaping using this design method. Furthermore, they developed an analytical method that can approximate the optical properties of metasurfaces without complex electromagnetic simulations. This analytical platform proposes a more intuitive and comprehensively applicable metasurface design guideline. The proposed technology is expected to enable accurate wavefront shaping with a much higher spatial resolution than existing wavefront shaping technologies, which will be applied to active optical systems such as mid-infrared holography, high-speed beam steering devices that can be applied for LiDAR, and variable focus infrared lenses. Professor Min Seok Jang commented, "This study showed the independent control amplitude and phase of light, which has been a long-standing quest in light modulator technology. The development of optical devices using complex wavefront control is expected to become more active in the future." MS candidate Sangjun Han and Dr. Seyoon Kim of the University of Wisconsin-Madison are the co-first authors of the research, which was published and selected as the front cover of the January 28 edition of ACS Nano titled “Complete complex amplitude modulation with electronically tunable graphene plasmonic metamolecules.” This research was funded by the Samsung Research Funding & Incubation Center for Future Technology. Publication: Han et al. (2020) Complete Complex Amplitude Modulation with Electronically Tunable Graphene Plasmonic Metamolecules. ACS Nano, Vol. 14, Issue 1, pp. 1166-1175. Available online at https://doi.org/10.1021/acsnano.9b09277 Profile: Prof. Min Seok Jang, MS, PhD firstname.lastname@example.org http://jlab.kaist.ac.kr/ Associate Professor Jang Research Group School of Electrical Engineering Korea Advanced Institute of Science and Technology (KAIST) http://kaist.ac.kr Daejeon, Republic of Korea Profile: Sangjun Han email@example.com MS Candidate School of Electrical Engineering Korea Advanced Institute of Science and Technology (KAIST) http://kaist.ac.kr Daejeon, Republic of Korea (END)
Wafer-Scale Multilayer Fabrication of Silk Fibroin-Based Microelectronics
A KAIST research team developed a novel fabrication method for the multilayer processing of silk-based microelectronics. This technology for creating a biodegradable silk fibroin film allows microfabrication with polymer or metal structures manufactured from photolithography. It can be a key technology in the implementation of silk fibroin-based biodegradable electronic devices or localized drug delivery through silk fibroin patterns. Silk fibroins are biocompatible, biodegradable, transparent, and flexible, which makes them excellent candidates for implantable biomedical devices, and they have also been used as biodegradable films and functional microstructures in biomedical applications. However, conventional microfabrication processes require strong etching solutions and solvents to modify the structure of silk fibroins. To prevent the silk fibroin from being damaged during the process, Professor Hyunjoo J. Lee from the School of Electrical Engineering and her team came up with a novel process, named aluminum hard mask on silk fibroin (AMoS), which is capable of micropatterning multiple layers composed of both fibroin and inorganic materials, such as metal and dielectrics with high-precision microscale alignment. The AMoS process can make silk fibroin patterns on devices, or make patterns on silk fibroin thin films with other materials by using photolithography, which is a core technology in the current microfabrication process. The team successfully cultured primary neurons on the processed silk fibroin micro-patterns, and confirmed that silk fibroin has excellent biocompatibility before and after the fabrication process and that it also can be applied to implanted biological devices. Through this technology, the team realized the multilayer micropatterning of fibroin films on a silk fibroin substrate and fabricated a biodegradable microelectric circuit consisting of resistors and silk fibroin dielectric capacitors in a silicon wafer with large areas. They also used this technology to position the micro-pattern of the silk fibroin thin film closer to the flexible polymer-based brain electrode, and confirmed the dye molecules mounted on the silk fibroin were transferred successfully from the micropatterns. Professor Lee said, “This technology facilitates wafer-scale, large-area processing of sensitive materials. We expect it to be applied to a wide range of biomedical devices in the future. Using the silk fibroin with micro-patterned brain electrodes can open up many new possibilities in research on brain circuits by mounting drugs that restrict or promote brain cell activities.” This research, in collaboration with Dr. Nakwon Choi from KIST and led by PhD candidate Geon Kook, was published in ACS AMI (10.1021/acsami.8b13170) on January 16, 2019. Figure 1. The cover page of ACS AMI Figure 2. Fibroin microstructures and metal patterns on a fibroin produced by using the AMoS mask. Figure 3. Biocompatibility assessment of the AMoS Process. Top: Schematics image of a) fibroin-coated silicon b) fibroin-pattered silicon and c) gold-patterned fibroin. Bottom: Representative confocal microscopy images of live (green) and dead (red) primary cortical neurons cultured on the substrates.
Developing Flexible Vertical Micro LED
A KAIST research team led by Professor Keon Jae Lee from the Department of Materials Science and Engineering and Professor Daesoo Kim from the Department of Biological Sciences has developed flexible vertical micro LEDs (f-VLEDs) using anisotropic conductive film (ACF)-based transfer and interconnection technology. The team also succeeded in controlling animal behavior via optogenetic stimulation of the f-VLEDs. Flexible micro LEDs have become a strong candidate for the next-generation display due to their ultra-low power consumption, fast response speed, and excellent flexibility. However, the previous micro LED technology had critical issues such as poor device efficiency, low thermal reliability, and the lack of interconnection technology for high-resolution micro LED displays. The research team has designed new transfer equipment and fabricated a f-VLED array (50ⅹ50) using simultaneous transfer and interconnection through the precise alignment of ACF bonding process. These f-VLEDs (thickness: 5 ㎛, size: below 80 ㎛) achieved optical power density (30 mW/mm2) three times higher than that of lateral micro LEDs, improving thermal reliability and lifetime by reducing heat generation within the thin film LEDs. These f-VLEDs can be applied to optogenetics for controlling the behavior of neuron cells and brains. In contrast to the electrical stimulation that activates all of the neurons in brain, optogenetics can stimulate specific excitatory or inhibitory neurons within the localized cortical areas of the brain, which facilitates precise analysis, high-resolution mapping, and neuron modulation of animal brains. (Refer to the author’s previous ACS Nano paper of “Optogenetic Mapping of Functional Connectivity in Freely Moving Mice via Insertable Wrapping Electrode Array Beneath the Skull.” ) In this work, they inserted the innovative f-VLEDs into the narrow space between the skull and the brain surface and succeeded in controlling mouse behavior by illuminating motor neurons on two-dimensional cortical areas located deep below the brain surface. Professor Lee said, “The flexible vertical micro LED can be used in low-power smart watches, mobile displays, and wearable lighting. In addition, these flexible optoelectronic devices are suitable for biomedical applications such as brain science, phototherapeutic treatment, and contact lens biosensors.” He recently established a startup company ( FRONICS Inc. ) based on micro LED technology and is looking for global partnerships for commercialization. This result entitled “ Optogenetic Control of Body Movements via Flexible Vertical Light-Emitting Diodes on Brain Surface ” was published in the February 2018 issue of Nano Energy. Figure 1. Comparison of μ-LEDs Technology
Innovative Nanosensor for Disease Diagnosis
(Figure 1. Sensing Device) (Figure 2. Protein templating route) Breath pattern recognition is a futuristic diagnostic platform. Simple characterizing target gas concentrations of human exhaled breath will lead to diagnose of the disease as well as physical condition. A research group under Prof. Il-Doo Kim in the Department of Materials Science has developed diagnostic sensors using protein-encapsulated nanocatalysts, which can diagnose certain diseases by analyzing human exhaled breath. This technology enables early monitoring of various diseases through pattern recognition of biomarker gases related to diseases in human exhalation. The protein-templated catalyst synthesis route is very simple and versatile for producing not only a single component of catalytic nanoparticles, but also diverse heterogeneous intermetallic catalysts with sizes less than 3 nm. The research team has developed ever more sensitive and selective chemiresistive sensors that can potentially diagnose specific diseases by analyzing exhaled breath gases. The results of this study, which were contributed by Dr. Sang-Joon Kim and Dr. Seon-Jin Choi as first authors were selected as the cover-featured article in the July issue of 'Accounts of Chemical Research,' an international journal of the American Chemical Society. In human breath, diverse components are found including water vapor, hydrogen, acetone, toluene, ammonia, hydrogen sulfide, and carbon monoxide, which are more excessively exhaled from patients. Some of these components are closely related to diseases such as asthma, lung cancer, type 1 diabetes mellitus, and halitosis. Breath analysis for disease diagnosis started from capturing exhaled breaths in a Tedlar bag and subsequently the captured breath gases were injected into a miniaturized sensor system, similar to an alcohol detector. It is possible to analyze exhaled breath very rapidly with a simple analyzing process. The breath analysis can detect trace changes in exhaled breath components, which contribute to early diagnosis of diseases. However, technological advances are needed to accurately analyze gases in the breath, which occur at very low levels, from 1 ppb to 1 ppm. In particular, it has been a critical challenge for chemiresistive type chemical sensors to selectively detect specific biomarkers in thousands of interfering gases including humid vapor. Conventionally, noble metallic catalysts such as platinum and palladium have been functionalized onto metal oxide sensing layers. However, the gas sensitivity was not enough to detect ppb-levels of biomarker species in exhaled breath. To overcome the current limitations, the research team utilized nanoscale protein (apoferritin) in animals as sacrificial templates. The protein templates possess hollow nanocages at the core site and various alloy catalytic nanoparticles can be encapsulated inside the protein nanocages. The protein nanocages are advantageous because a nearly unlimited number of material compositions in the periodic table can be assembled for the synthesis of heterogeneous catalytic nanoparticles. In addition, intermetallic nanocatalysts with a controlled atomic ratio of two different elements can be achieved using the protein nanocages, which is an innovative strategy for finding new types of catalysts. For example, highly efficient platinum-based catalysts can be synthesized, such as platinum-palladium (PtPd), platinum-nickel (PtNi), platinum-ruthenium (PtRu), and platinum-yttrium (PtY). The research team developed outstanding sensing layers consisting of metal oxide nanofibers functionalized by the heterogeneous catalysts with large and highly-porous surface areas, which are especially optimized for selective detection of specific biomarkers. The biomarker sensing performance was improved approximately 3~4-fold as compared to the conventional single component of platinum and palladium catalysts-loaded nanofiber sensors. In particular, 100-fold resistance transitions toward acetone (1 ppm) and hydrogen sulfide (1 ppm) were observed in exhaled breath sensors using the heterogeneous nanocatalysts, which is the best performance ever reported in literature. The research team developed a disease diagnosis platform that recognizes individual breathing patterns by using a multiple sensor array system with diverse sensing layers and heterogeneous catalysts, so that the people can easily identify health abnormalities. Using a 16-sensor array system, physical conditions can be continuously monitored by analyzing concentration changes of biomarkers in exhaled breath gases. Prof. Kim said, “New types of heterogeneous nanocatalysts were synthesized using protein templates with sizes around 2 nm and functionalized on various metal oxide nanofiber sensing layers. The established sensing libraries can detect biomarker species with high sensitivity and selectivity.” He added, “the new and innovative breath gas analysis platform will be very helpful for reducing medical expenditures and continuous monitoring of physical conditions” Patents related to this technology were licensed to two companies in March and June this year.
Total Synthesis of Flueggenine C via an Accelerated Intermolecular Rauhut-Currier Reaction
The first total synthesis of dimeric securinega alkaloid (-)-flueggenine C was completed via an accelerated intermolecular Rauhut–Currier (RC) reaction. The research team led by Professor Sunkyu Han in the Department of Chemistry succeeded in synthesizing the natural product by reinventing the conventional RC reaction. The total synthesis of natural products refers to the process of synthesizing secondary metabolites isolated from living organisms in the laboratory through a series of chemical reactions. Each stage of chemical reaction needs to be successful to produce the final target molecule, and thus the process requires high levels of patience and creativity. For that reason, the researchers working on natural products total synthesis are often called “molecular artists”. Despite numerous reports on the total synthesis of monomeric securinegas, the synthesis of dimeric securinegas, whose monomeric units are connected by a putative enzymatic RC reaction, has not been reported to date. The team used a Rauhut-Currier (RC) reaction, a carboncarbon bond forming a reaction between two Michael acceptors first reported by Rauhut and Currier in 1963, to successfully synthesize a dimeric natural product, flueggenine C. This new work featured the first application of an intermolecular RC reaction in total synthesis. The conventional intermolecular RC reaction was driven non-selectively by a toxic nucleophilic catalyst at a high temperature of over 150°C and a highly concentrated reaction mixture, and thus has never been applied to natural products total synthesis. To overcome this long-standing problem, the research team placed a nucleophilic moiety at the γ-position of the enone derivative. As a result, the RC reaction could be induced by the simple addition of a base at ambient temperature and dilute solution, without the need of a nucleophilic catalyst. Using this newly discovered reactivity, the team successfully synthesized the natural product (-)-flueggenine C from commercially available amino acid derivative in 12 steps. Professor Han said, “Our key finding regarding the remarkably improved reactivity and selectivity of the intermolecular RC reaction will serve as a significant stepping stone in allowing this reaction to be considered a practical and reliable chemical tool with broad applicability in natural products, pharmaceuticals, and materials syntheses. ” This research was led by Ph.D. candidate Sangbin Jeon and was published in The Journal of the American Chemical Society (JACS) on May 10. This research was funded by KAIST start-up funds, HRHR (High-Risk High-Return), RED&B (Research, Education, Development & Business) projects, the National Research Foundation of Korea, and the Institute for Basic Science. (Figure 1: Representative dimeric/oligomeric securinega alkaloids) (Figure 2: Our reinvented Rauhut-Currier reaction) (Figure 3: Total Synthesis of (-)-flueggenine C)
Gout Diagnostic Strip Using a Single Teardrop
A novel diagnostic strip for gout patients using a single teardrop has been announced by KAIST research team. This technology analyzes biological molecules in tears for a non-invasive diagnosis, significantly reducing the time and expense previously required for a diagnosis. The research team under Professor Ki-Hun Jeong of the Department of Bio and Brain Engineering succeeded in developing an affordable and elaborate gout diagnostic strip by depositing metal nanoparticles on paper. This technology can not only be used in diagnostic medicine and drug testing, but also in various other areas such as field diagnoses that require prompt and accurate detection of a certain substance. Gout induces pain in joints due to needle-shaped uric acid crystal build up. In general, therapeutic treatments exist to administer pain relief, stimulate uric acid discharge, and uric acid depressant. Such treatments work for temporary relief, but there have significant limitations. Thus, patients are required to regularly check uric acid concentrations, as well as control their diets. Therefore, simpler ways to measure uric acid would greatly benefit gout control and its prevention in a more affordable and convenient manner. Existing gout diagnostic techniques include measuring uric acid concentrations from blood samples or observing uric acid crystals from joint synovial fluid under a microscope. These existing methods are invasive and time consuming. To overcome their limitations, the research team uniformly deposited gold nanoislands with nanoplasnomics properties on the surface of paper that can easily collect tears. Nanoplasnomics techniques collect light on the surface of a metal nanostructure, and can be applied to disease and health diagnostic indicators as well as for genetic material detection. Further, metals such as gold absorb stronger light when it is irradiated, and thus can maximize light concentration on board surfaces while maintaining the properties of paper. The developed metal nanostructure production technology allows the flexible manufacturing of nanostructures on a large surface, which in turn allows flexible control of light concentrations. The research team grafted surface-enhanced Raman spectroscopy on paper diagnostic strips to allow uric acid concentration measurements in teardrops without additional indicators. The measured concentration in teardrops can be compared to blood uric acid concentrations for diagnosing gout. Professor Jeong explained, “Based on these research results, our strip will make it possible to conduct low-cost, no indicator, supersensitive biological molecule analysis and fast field diagnosis using tears.” He continued, “Tears, as well as various other bodily fluids, can be used to contribute to disease diagnosis and physiological functional research.” Ph.D. candidate Moonseong Park participated in the research as the first author of the paper that was published in the online edition of ACS Nano on December 14, 2016. Park said, “The strip will allow fast and simple field diagnosis, and can be produced on a large scale using the existing semiconductor process.” (Figure 1. Optical image of paper gout diagnostic strip covered with gold) (Figure 2. Scanning delectron microscopic image of paper gout diagnostic strip) (Figure 3. Scanning electron microscope image of cellulos fiber coated with gold nanoislands) (Figure 4. Gout diagnosis using tears)
A Transport Technology for Nanowires Thermally Treated at 700 Celsius Degrees
Professor Jun-Bo Yoon and his research team of the Department of Electrical Engineering at KAIST developed a technology for transporting thermally treated nanowires to a flexible substrate and created a high performance device for collecting flexible energy by using the new technology. Mr. Min-Ho Seo, a Ph.D. candidate, participated in this study as the first author. The results were published online on January 30th in ACS Nano, an international journal in the field of nanoscience and engineering. (“Versatile Transfer of an Ultralong and Seamless Nanowire Array Crystallized at High Temperature for Use in High-performance Flexible Devices,” DOI: 10.1021/acsnano.6b06842) Nanowires are one of the most representative nanomaterials. They have wire structures with dimensions in nanometers. The nanowires are widely used in the scientific and engineering fields due to their prominent physical and chemical properties that depend on a one-dimensional structure, and their high applicability. Nanowires have much higher performance if their structure has unique features such as an excellent arrangement and a longer-than-average length. Many researchers are thus actively participating in the research for making nanowires without much difficulty, analyzing them, and developing them for high performance application devices. Scientists have recently favored a research topic on making nanowires chemically and physically on a flexible substrate and applies the nanowires to a flexible electric device such as a high performance wearable sensor. The existing technology, however, mixed nanowires from a chemical synthesis with a solution and spread the mixture on a flexible substrate. The resultant distribution was random, and it was difficult to produce a high performance device based on the structural advantages of nanowires. In addition, the technology used a cutting edge nano-process and flexible materials, but this was not economically beneficial. The production of stable materials at a temperature of 700 Celsius degrees or higher is unattainable, a great challenge for the application. To solve this problem, the research team developed a new nano-transfer technology that combines a silicon nano-grating board with a large surface area and a nano-sacrificial layer process. A nano-sacrificial layer exists between nanowires and a nano-grating board, which acts as the mold for the nano-transfer. The new technology allows the device undergo thermal treatment. After this, the layer disappears when the nanowires are transported to a flexible substrate. This technology also permits the stable production of nanowires with secured properties at an extremely high temperature. In this case, the nanowires are neatly organized on a flexible substrate. The research team used the technology to manufacture barium carbonate nanowires on top of the flexible substrate. The wires secured their properties at a temperature of 700℃ or above. The team employed the collection of wearable energy to obtain much higher electrical energy than that of an energy collecting device designed based on regular barium titanate nanowires. The researchers said that their technology is built upon a semiconductor process, known as Physical Vapor Deposition that allows various materials such as ceramics and semiconductors to be used for flexible substrates of nanowires. They expected that high performance flexible electric devices such as flexible transistors and thermoelectric elements can be produced with this method. Mr. Seo said, “In this study, we transported nanowire materials with developed properties on a flexible substrate and showed an increase in device performance. Our technology will be fundamental to the production of various nanowires on a flexible substrate as well as the feasibility of making high performance wearable electric devices.” This research was supported by the Leap Research Support Program of the National Research Foundation of Korea. Fig. 1. Transcription process of new, developed nanowires (a) and a fundamental mimetic diagram of a nano-sacrificial layer (b) Fig. 2. Transcription results from using gold (AU) nanowires. The categories of the results were (a) optical images, (b) physical signals, (c) cross-sectional images from a scanning electron microscope (SEM), and (d-f) an electric verification of whether the perfectly arranged nanowires were made on a large surface. Fig. 3. Transcription from using barium titanate (BaTiO3) nanowires. The results were (a) optical images, (b-e) top images taken from an SEM in various locations, and (f, g) property analysis. Fig. 4. Mimetic diagram of the energy collecting device from using a BaTiO3 nanowire substrate and an optical image of the experiment for the miniature energy collecting device attached to an index finger.
Quantum Dot Film Can Withstand High Temperatures and Humidity
The joint KAIST research team of Professor Byeong-Soo Bae of the Department of Materials Science and Engineering and Professor Doh Chang Lee of the Department of Chemical and Biomolecular Engineering was able to fabricate a siloxane-encapsulated quantum dot film, which exhibits stable emission intensity over one month even at high temperatures and humidity. The results of this study were published in the Journal of the American Chemical Society (JACS) on November 29, 2016. The research article is entitled “Quantum Dot/Siloxane Composite Film Exceptionally Stable against Oxidation under Heat and Moisture.” (DOI: 10.1021/jacs.6b10681) Quantum dots (QDs), light-emitting diodes (LEDs) for next-generation displays, are tiny particles or nanocrystals of semiconducting materials. Their emission wavelength can easily be adjusted by changing their sizes, which are just a few nanometers. A wide spectrum of their colors can also achieve ultra-high definition displays. Due to these characteristics, QDs are coated on a film as a polymer resin in dispersed form, or they are spread on an LED light source. They are thus considered to be crucial for next generation displays. Despite their exceptional optical properties, however, QDs are easily oxidized in a high temperature and high humidity environment, and, as a result, this greatly deteriorates their luminescence quality (quantum efficiency). Therefore, they are encapsulated in an extra thin layer to block oxygen and moisture. QD displays in the current market have a film inserted to separate them from LEDs, which create heat. The high unit cost of this protective layer, however, increases the overall cost of displays, lowering their price competitiveness in the market. For a solution, the research team applied the sol-gel condensation reaction of silane precursors with QDs. This technology uses the reactions of chemical substances to synthesize ceramics or glass at a low temperature. The team applied QDs in a heat resistant siloxane polymer by employing this technology. The siloxane resin acted as a cup holding the QDs and also blocked heat and moisture. Thus, their performance can be maintained without an extra protective film. QDs are evenly dispersed into the resin from a chemical process to fabricate a QD embedded film and retained the high quality luminescence not only at a high temperature of 85°C and in a high humidity of 85%, but also in a high acid and high base environment. Remarkably though, the luminescence actually increased in the high humidity environment. If this technology is used, the overall price of displays will decrease by producing a stable QD film without an extra protective barrier. In the future, the QD film can be directly applied to a blue LED light source. As a result, it will be possible to develop a QD display that can reduce the amount of QDs needed and improve its performance. Professor Bae said, “We have proposed a way to make quantum dots overcome their limitations and have wide applications as they are being developed for next-generation displays. Our technology will make significant contributions to the display industry in the country.” He also added, “In the future, we plan to cooperate with companies both in and out of the country to improve the performance of quantum dots and concentrate on their commercialization.” The research team is currently applying for related patents both in and out of the country. The team is also plan ning to transfer the patents to Sol Ip Technology Inc., a company founded at KAIST, to start the commercialization. Picture 1: Siloxane-encapsulated quantum dot (QD) films showing performance stability in boiling water Picture 2 and 3: So-gel condensation reaction in silane precursors between Methacryloxypropyltrimethoxysilane (MPTS) and diphenylsilanediol (DPSD). The inset shows photographs of a QD-oligosiloxane resin under room light (left) and a UV lamp (λ = 365 nm) (right). Free radical addition reactions among carbon double bonds of methacryl functional groups and oleic acids. The inset shows photographs of a QD-silox film under room light (left) and a UV lamp (λ = 365 nm) (right).
An Improved Carbon Nanotube Semiconductor
Professor Yang-Kyu Choi and his research team of the School of Electrical Engineering at KAIST collaborated with Professor Sung-Jin Choi of Kookmin University to develop a large-scale carbon nanotube semiconductor by using a 3-D fin-gate structure with carbon nanotubes on its top. Dong Il Lee, a postdoctoral researcher at KAIST’s Electrical Engineering School, participated in this study as the first author. It was published in ACS Nano on November 10, 2016, and was entitled “Three-Dimensional Fin-Structured Semiconducting Carbon Nanotube Network Transistor.” A semiconductor made with carbon nanotubes operates faster than a silicon semiconductor and requires less energy, yielding higher performance. Most electronic equipment and devices, however, use silicon semiconductors because it is difficult to fabricate highly purified and densely packed semiconductors with carbon nanotubes (CNTs). To date, the performance of CNTs was limited due to their low density. Their purity was also low, so it was impossible to make products that had a constant yield on a large-surface wafer or substrate. These characteristics made the mass production of semiconducting CNTs difficult. To solve these difficulties, the research team used a 3-D fin-gate to vapor-deposit carbon nanotubes on its top. They developed a semiconductor that had a high current density with a width less than 50 nm. The three-dimensional fin structure was able to vapor-deposit 600 carbon nanotubes per micrometer. This structure could have 20 times more nanotubes than the two dimensional structure, which could only vapor-deposit thirty in the same 1 micrometer width. In addition, the research team used semi-conductive carbon nanotubes having a purity rating higher than 99.9% from a previous study to obtain a high yield semiconductor. The semiconductor from the research group has a high current density even with a width less than 50 μm. The new semiconductor is expected to be five times faster than a silicon-based semiconductor and will require five times less electricity during operation. Furthermore, the new semiconductor can be made by or will be compatible with the equipment for producing silicon-based semiconductors, so there will be no additional costs. Researcher Lee said, “As a next generation semiconductor, the carbon nanotube semiconductor will have better performance, and its effectiveness will be higher.” He also added, “Hopefully, the new semiconductor will replace the silicon-based semiconductors in ten years.” This study received support from the Center for Integrated Smart Sensors funded by the Ministry of Science, ICT & Future Planning of Korea as the Global Frontier Project, and from the CMOS (Complementary Metal-Oxide-Semiconductor) THz Technology Convergence Center of the Pioneer Research Center Program sponsored by the National Research Foundation of Korea. Picture 1: 3D Diagram of the Carbon Nanotube Electronic Device and Its Scanning Electron Microscope (SEM) Image Picture 2: 3D Transistor Device on an 8-inch Base and the SEM Image of Its Cross Section
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