Ji Hyun An

High-Performance Flexible Graphene Aptasensor for Mercury Detection in Mussels

Mercury (Hg) is highly toxic but has been widely used for numerous domestic applications, including thermometers and batteries, for decades, which has led to fatal outcomes due to its accumulation in the human body. Although many types of mercury sensors have been developed to protect the users from Hg, few methodologies exist to analyze Hg(2+) ions in low concentrations in real world samples. Herein, we describe the fabrication and characterization of liquid-ion gated field-effect transistor (FET)-type flexible graphene aptasensor with high sensitivity and selectivity for Hg. The field-induced responses from the graphene aptasensor had excellent sensing performance, and Hg(2+) ions with very low concentration of 10 pM could be detected, which is 2-3 orders of magnitude more sensitive than previously reported mercury sensors using electrochemical systems. Moreover, the aptasensor showed a highly specific response to Hg(2+) ions in mixed solutions. The flexible graphene aptasensor showed a very rapid response, providing a signal in less than 1 s when the Hg(2+) ion concentration was altered. Specificity to Hg(2+) ions was demonstrated in real world samples (in this case samples derived from mussels). The aptasensor was fabricated by transferring chemical vapor deposition (CVD)-grown graphene onto a transparent flexible substrate, and the structure displayed excellent mechanical durability and flexiblility. This graphene-based aptasensor has potential for detecting Hg exposure in human and in the environment.

Large‐Scale Graphene Micropattern Nano‐biohybrids: High‐Performance Transducers for FET‐Type Flexible Fluidic HIV Immunoassays

Large-scale FET-type graphene micropattern (GM) nano-biohybrid-based immunosensor (GMNS) is fabricated in a controlled fashion to detect human immunodeficiency virus 2 antibody. Flexible GMNS shows a highly sensitive response and excellent mechanical bendability. The flexible GMNS in fluidic systems also has a stable response. This is the first experimental demonstration of a large-scale flexible fluidic FET-type immunoassay based on GM nano-biohybrids.

An Ultrasensitive, Selective, Multiplexed Superbioelectronic Nose That Mimics the Human Sense of Smell

Human sensory-mimicking systems, such as electronic brains, tongues, skin, and ears, have been promoted for use in improving social welfare. However, no significant achievements have been made in mimicking the human nose due to the complexity of olfactory sensory neurons. Combinational coding of human olfactory receptors (hORs) is essential for odorant discrimination in mixtures, and the development of hOR-combined multiplexed systems has progressed slowly. Here, we report the first demonstration of an artificial multiplexed superbioelectronic nose (MSB-nose) that mimics the human olfactory sensory system, leading to high-performance odorant discriminatory ability in mixtures. Specifically, portable MSB-noses were constructed using highly uniform graphene micropatterns (GMs) that were conjugated with two different hORs, which were employed as transducers in a liquid-ion gated field-effect transistor (FET). Field-induced signals from the MSB-nose were monitored and provided high sensitivity and selectivity toward target odorants (minimum detectable level: 0.1 fM). More importantly, the potential of the MSB-nose as a tool to encode hOR combinations was demonstrated using principal component analysis.

Flower-like Palladium Nanoclusters Decorated Graphene Electrodes for Ultrasensitive and Flexible Hydrogen Gas Sensing

Flower-like palladium nanoclusters (FPNCs) are electrodeposited onto graphene electrode that are prepared by chemical vapor deposition (CVD). The CVD graphene layer is transferred onto a poly(ethylene naphthalate) (PEN) film to provide a mechanical stability and flexibility. The surface of the CVD graphene is functionalized with diaminonaphthalene (DAN) to form flower shapes. Palladium nanoparticles act as templates to mediate the formation of FPNCs, which increase in size with reaction time. The population of FPNCs can be controlled by adjusting the DAN concentration as functionalization solution. These FPNCs_CG electrodes are sensitive to hydrogen gas at room temperature. The sensitivity and response time as a function of the FPNCs population are investigated, resulted in improved performance with increasing population. Furthermore, the minimum detectable level (MDL) of hydrogen is 0.1 ppm, which is at least 2 orders of magnitude lower than that of chemical sensors based on other Pd-based hybrid materials.

Human dopamine receptor nanovesicles for gate-potential modulators in high-performance field-effect transistor biosensors.

The development of molecular detection that allows rapid responses with high sensitivity and selectivity remains challenging. Herein, we demonstrate the strategy of novel bio-nanotechnology to successfully fabricate high-performance dopamine (DA) biosensor using DA Receptor-containing uniform-particle-shaped Nanovesicles-immobilized Carboxylated poly(3,4-ethylenedioxythiophene) (CPEDOT) NTs (DRNCNs). DA molecules are commonly associated with serious diseases, such as Parkinsons and Alzheimers diseases. For the first time, nanovesicles containing a human DA receptor D1 (hDRD1) were successfully constructed from HEK-293 cells, stably expressing hDRD1. The nanovesicles containing hDRD1 as gate-potential modulator on the conducting polymer (CP) nanomaterial transistors provided high-performance responses to DA molecule owing to their uniform, monodispersive morphologies and outstanding discrimination ability. Specifically, the DRNCNs were integrated into a liquid-ion gated field-effect transistor (FET) system via immobilization and attachment processes, leading to high sensitivity and excellent selectivity toward DA in liquid state. Unprecedentedly, the minimum detectable level (MDL) from the field-induced DA responses was as low as 10 pM in real- time, which is 10 times more sensitive than that of previously reported CP based-DA biosensors. Moreover, the FET-type DRNCN biosensor had a rapid response time (<1 s) and showed excellent selectivity in human serum.

Duplex Bioelectronic Tongue for Sensing Umami and Sweet Tastes Based on Human Taste Receptor Nanovesicles

For several decades, significant efforts have been made in developing artificial taste sensors to recognize the five basic tastes. So far, the well-established taste sensor is an E-tongue, which is constructed with polymer and lipid membranes. However, the previous artificial taste sensors have limitations in various food, beverage, and cosmetic industries because of their failure to mimic human taste reception. There are many interactions between tastants. Therefore, detecting the interactions in a multiplexing system is required. Herein, we developed a duplex bioelectronic tongue (DBT) based on graphene field-effect transistors that were functionalized with heterodimeric human umami taste and sweet taste receptor nanovesicles. Two types of nanovesicles, which have human T1R1/T1R3 for the umami taste and human T1R2/T1R3 for the sweet taste on their membranes, immobilized on micropatterned graphene surfaces were used for the simultaneous detection of the umami and sweet tastants. The DBT platform led to highly sensitive and selective recognition of target tastants at low concentrations (ca. 100 nM). Moreover, our DBT was able to detect the enhancing effect of taste enhancers as in a human taste sensory system. This technique can be a useful tool for the detection of tastes instead of sensory evaluation and development of new artificial tastants in the food and beverage industry.

Size-controllable ultrathin carboxylated polypyrrole nanotube transducer for extremely sensitive 17β-estradiol FET-type biosensors

17β-Estradiol is known as a steroid hormone in the human body but it is also known as a disruptor that can cause disequilibrium and dysfunction of the human immune system. Recently, there has been much interest in developing biosensors to detect low concentrations of 17β-estradiol. In this work, size-controllable aptamer conjugated ultrathin carboxylated polypyrrole nanotubes (A-UCPPyNTs) were fabricated as transducers in 17β-estradiol field-effect transistor (FET)-type biosensors. They were manufactured via a self-degradation method under several different conditions to control the diameter of the nanotubes. For targeting 17β-estradiol, the binding aptamers were immobilized through covalent bonding on its surface. The resulting A-UCPNT FET-type biosensor demonstrated p-type behavior with outstanding electrical conductivity, and exhibited Ohmic contacts between the samples and electrodes. The smaller diameter (40 nm) of ultrathin carboxylated polypyrrole nanotubes (UCPPyNTs) contributed to the biosensors enhanced performance by generating a larger surface area, thereby increasing the number of conjugated binding aptamers. In conclusion, the A-UCPPyNT FET-type biosensor showed extremely high sensitivity (∼1 fM) toward 17β-estradiol, approximately 103 times more sensitive than the results found in other reports. Moreover, the A-UCPPyNT FET-type biosensor showed unique selectivity to the 17β-estradiol molecule, in addition to outstanding reusability and long-term storage stability (4 weeks of duration achieved in this work). These performances concerned with reusability and stability were achieved by the formation of covalent bonding in the anchorage to the substrate electrode. Thus this study can be effectively applied in biological and environmental fields.

Multidimensional Conductive Nanofilm-Based Flexible Aptasensor for Ultrasensitive and Selective HBsAg Detection

Hepatitis B virus (HBV) infection is a major worldwide health issue causing serious liver diseases, including liver cirrhosis and hepatocellular carcinoma. Monitoring the serum hepatitis B surface antigen (HBsAg) level is pivotal to the diagnosis of HBV infection. In this study, we describe multidimensional conductive nanofilm (MCNF)-based field-effect transistor (FET) aptasensor for HBsAg detection. The MCNF, composed of vertically oriented carboxylic polypyrrole nanowires (CPPyNW) and graphene layer, is formed using electropolymerization of pyrrole on the graphene surface and following acid treatment. The amine-functionalized HBsAg-binding aptamers are then immobilized on the CPPyNW surface through covalent bonding formation (i.e., amide group). The prepared aptasensor presents highly sensitive to HBsAg as low as 10 aM among interfering biomolecules with various deformations. Moreover, the MCNF-based aptasensor has great potential for practical application in the noninvasive real-time diagnosis because of its improved sensing ability to the human serum and artificial saliva.