Chemistry / Kimya
Permanent URI for this collectionhttps://hdl.handle.net/11147/4072
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Article Free-Standing Three-Dimensional Graphene Scaffolds for Protease Functional Assay(Elsevier Science Sa, 2024) Ng, Zhi Kai; Yan, Evelias; Goyal, Garima; Gudlur, Sushanth; Kanagavel, Deepankumar; Yildiz, Umit Hakan; Teo, Edwin Hang TongThree-dimensional graphene scaffolds (3d-GS) of high porosity possessing good fluorescence quenching properties are potential candidates for the development of optical biosensors. Herein, we demonstrate the feasibility of utilising intact and free-standing 3d-GS for sensitive detection of proteases, a class of disease diagnosis bio-markers of significant interest. Recombinant OmpT was employed as a model protease for validating the pro-posed methodology. A short (15-residue) peptide sequence encoding a specific recognition site for OmpT was end-labelled with a fluorescent dye (5-FAM) whose fluorescence is quenched when the peptide is anchored to 3d-GS. However, in the presence of OmpT, the peptide is cleaved and released from 3d-GS, resulting in a sig-nificant recovery in fluorescence. The functional assay described herein involves a single step fabrication process of anchoring the peptide to 3d-GS. The integrity of the 3d-GS is hypothesised to overcome the concern of dynamic requenching associated with the typical homogeneous assays based on graphene, yielding a limit of detection (LOD) of similar to 140 nM, which is over an order higher than homogeneous assays performed using the same composition of graphene in powdered form. To the best of our knowledge, this is the first report on utilising free-standing 3d-GS for facile assaying of proteases.Conference Object Citation - WoS: 3Citation - Scopus: 3Halloysite Nanotube Loaded Polyamide Nanocomposites: Structural, Morphological, Mechanical, Thermal and Processing Behaviors(American Institute of Physics, 2023) Akar, Alinda Öykü; Yıldız, Ümit Hakan; Tayfun, ÜmitIn this study, the polyamide 6 (PA) matrix was reinforced with the purified, fine ground and amino-silane treated halloysite nanotubes (HNT) at different concentrations. The preparation of composites was carried out using a lab-scale twin-screw micro-compounder with loading ratios at 0.5, 1, 3, and 20% by weight, and the test samples were prepared by the injection-molding process. According to mechanical test results, additions of HNT to the PA matrix caused slight improvements in tensile strength and Youngs' modulus parameters. The optimum concentrations for all of the additives used were estimated by comparison of mechanical test data. The addition of aminosilane-modified HNT resulted in a higher impact performance at high loading levels up to 3% concentrations. Further addition of HNT caused a reduction in the mechanical parameters of composites. Thermal studies revealed that the glass transition temperature of PA shifted to higher values after HNT mineral inclusions. Thermo-mechanical results showed that storage moduli of PA exhibited improvement with an increase in HNT content. The distributions of HNT clay into the PA phase were visualized with SEM images. Based on these observations, a high level of dispersion homogeneity was achieved for lower filling ratios. According to melt-flow and force measurements, composites filled with 20% of HNT displayed a remarkable increase in exerted force during melt-blending. © 2023 Author(s).Article Citation - WoS: 5Citation - Scopus: 4Polarity Induced Vapochromism and Vapoluminescence of Polythiophene Derivatives for Volatile Organic Compounds Classification(Elsevier, 2023) Karabacak, Soner; Qun, David Lee Chao; Ammanath, Gopal; Yeasmin, Sanjida; Yağmurcukardeş, Mehmet; Palaniappan, Alagappan; Liedberg, Bo; Yıldız, Ümit HakanPolarity induced vapochromic and vapoluminescent properties of cationic poly-3-alkoxythiophene derivatives (PT) casted on polyvinylidene fluoride (PVDF) membranes are reported. PT with six different pendant groups are designed to differentially interact with volatile organic compounds (VOC) of varying polarities, thereby enabling their classification. PT exhibit a rapid vapochromic response with a concurrent modulation of vapoluminescence due to the non-covalent cation-? interactions between the pendant groups and the PT backbone. Adsorption of VOC on pendant groups alters the conformation of PT backbone, thus resulting in an increase in intensity and blue shifting of fluorescence emission within the visible spectrum. The vapoluminescent responses are found to be more sensitive with a limit of detection (LOD) of ?7 ppm and a wider dynamic range as compared to the vapochromic responses with a LOD of ?60 ppm for the detection of a model VOC: chloroform. Notably, all the PT illustrate an instantaneous recovery of colour and luminescence upon desorption of VOC. PT interaction with VOC of varying polarities was ascertained using density functional theory (DFT) and principal component analysis (PCA) methodologies. In summary, the polarity induced vapochromic and vapoluminescent properties of PT could yield a selective and sensitive vapochromic and fluorometric dual-mode VOC detection platform. © 2023Article Citation - WoS: 1Citation - Scopus: 1A Multi-Layered Graphene Based Gas Sensor Platform for Discrimination of Volatile Organic Compounds Via Differential Intercalation(Royal Society of Chemistry, 2023) Özkendir İnanç, Dilce; Ng, Zhi Kai; Başkurt, Mehmet; Keleş, Berfin; Vardar, Gökay; Şahin, Hasan; Tsang, Siu Hon; Palaniappan, Alagappan; Yıldız, Ümit Hakan; Teo, EhtSelective and sensitive detection of volatile organic compounds (VOCs) is of critical importance for environmental monitoring, disease diagnosis and industrial applications. Among VOCs, assay development for primary alcohols has captured significant research attention since their toxicity causes adverse effects on gastrointestinal and central nerve systems, resulting in irreversible blindness, and coma, and can be even fatal at high exposure levels. However, selective detection of primary alcohols is extremely challenging owing to the similarity in their molecular structure and characteristic groups. Herein, we have attempted to investigate the differential methanol (MeOH)-ethanol (EtOH) discriminative properties of single-layer, bi-layer, and multi-layer graphene morphologies. Chemiresistors fabricated using the three morphologies of graphene illustrate discriminative MeOH-EtOH responses, which is attributed to the phenomenon of differential intercalation of MeOH within layered graphene morphologies as compared to that of EtOH. This hypothesis is verified by density functional theory calculations, which revealed that the adsorption of EtOH molecules on the graphene surface is more energetically favorable as compared to that of MeOH molecules, thereby inhibiting their intercalation within the layered graphene morphologies. It is further evaluated that the degree of MeOH intercalation increases with increasing layers of graphene for obtaining differential MeOH-EtOH responses. Experimental results suggest possibilities to develop selective and sensitive MeOH assays fabricated using various graphene morphologies in a combinatorial sensor array format.Article Citation - WoS: 4Citation - Scopus: 4Colorimetric Assaying of Exosomal Metabolic Biomarkers(MDPI, 2023) Yan, Evelias; Goyal, Garima; Yıldız, Ümit Hakan; Boehm, Bernhard O.; Palaniappan, AlagappanExosomes released into the extracellular matrix have been reported to contain metabolic biomarkers of various diseases. These intraluminal vesicles are typically found in blood, urine, saliva, breast milk, cerebrospinal fluid, semen, amniotic fluid, and ascites. Analysis of exosomal content with specific profiles of DNA, microRNA, proteins, and lipids can mirror their cellular origin and physiological state. Therefore, exosomal cargos may reflect the physiological processes at cellular level and can potentially be used as biomarkers. Herein, we report an optical detection method for assaying exosomal biomarkers that supersedes the state-of-the-art time consuming and laborious assays such as ELISA and NTA. The proposed assay monitors the changes in optical properties of poly(3-(4-methyl-3'-thienyloxy) propyltriethylammonium bromide) upon interacting with aptamers/peptide nucleic acids in the presence or absence of target biomarkers. As a proof of concept, this study demonstrates facile assaying of microRNA, DNA, and advanced glycation end products in exosomes isolated from human plasma with detection levels of ~1.2, 0.04, and 0.35 fM/exosome, respectively. Thus, the obtained results illustrate that the proposed methodology is applicable for rapid and facile detection of generic exosomal biomarkers for facilitating diseases diagnosis.Conference Object Citation - WoS: 1Citation - Scopus: 1Biomimetic Peptide-Conjugated Membranes for Developing an Artificial Cornea(IEEE, 2022) Sunal, Gülşah; Pulat, Günnur; Akgün, İsmail Hakkı; Güven, Sinan; Yıldız, Ümit Hakan; Karaman, Ozan; Horzum, NesrinThe corneal endothelium is composed of a single layer of specialized endothelial cells, protecting, and nourishing the inner surface of the cornea. Corneal endothelial cells do not proliferate after birth and their number decrease with age. Trauma, inflammation, or surgical intervention can cause cell loss. When damage is extensive and the density of corneal endothelial cells decreases to a critical level, it results in corneal edema and vision loss. Besides them, when corneal endothelium has irreversible damage, the only treatment way is corneal transplantation. But there are some drawbacks such as finding donors, immune reactions, and the number of patients waiting on the transplantation lists for years. Tissue engineering approaches can provide promising alternatives for the regeneration of corneal endothelium tissue. Peptides can be used to modify and functionalize the scaffolds, allowing for the production of bioactive and biomimetic surfaces. Peptide-modified scaffold surfaces might direct and enhance the behaviors of cells. In this study, the aim was to functionalize the polycaprolactone (PCL) membranes with tissue-specific peptides and to characterize the peptide-conjugated membranes by Fourier-Transform Infrared Spectroscopy (FTIR), Scanning Electron Microscopy (SEM), and X-ray Photoelectron Spectroscopy (XPS) analysis. The synthesized peptides were successfully conjugated on the PCL biomembranes.Article Citation - WoS: 35Citation - Scopus: 44Current Trends and Challenges in Point-Of Urinalysis of Biomarkers in Trace Amounts(Elsevier, 2022) Yeasmin, Sanjida; Ammanath, Gopal; Önder, Ahmet; Yan, Evelias; Yıldız, Ümit Hakan; Palaniappan, Alagappan; Liedberg, BoUrinalysis enables non-invasive point-of-care (POC) testing of numerous biomarkers at their physiological and elevated levels, obviating the need for sophisticated equipment or trained personnel. POC urinalysis is used to identify biomarkers that are rich in urine (greater than 1 μM), such as lactate, uric acid, glucose, ions, and adenosine. Urine also contains biomarkers such as small molecules, nucleic acids, neurotransmitters, and drugs in trace amounts (less than 1 μM). These biomarkers are of significant importance for health care monitoring, diagnosis of various disorders (cancer, metabolic diseases, etc.) and illicit drug control (cocaine, steroids, etc.). While POC detection of urinary biomarkers at higher concentration (μM to mM) levels is feasible, direct assaying of biomarkers in nM to fM levels is challenging, as assay responses are typically masked by interferences from the urine sample matrix. This report is a consolidated review of emerging trends and challenges in the POC urinalysis for detecting biomarkers that are less abundant in urine. The sensing mechanisms, analytical device fabrication, discrete and integrated sample pre-treatment procedures for POC assaying of urinary markers in trace amounts are elaborated. Subsequently, the utilization of smart data analytics for facilitating personalized urinalysis is presented. A comprehensive outlook on associated challenges in POC urinalysis of biomarkers in trace amounts is further provided, which would facilitate the advancement of POC urinalysis for a wide range of healthcare applications.Article Citation - WoS: 14Citation - Scopus: 19Influence of Carbon Nanotube Inclusions To Electrical, Thermal, Physical and Mechanical Behaviors of Carbon-Fiber Abs Composites(Springer, 2022) Akar, Alinda Öykü; Yıldız, Ümit Hakan; Tirkeş, Seha; Tayfun, Ümit; Hacıvelioğlu, FerdaAcrylonitrile–butadiene–styrene (ABS) terpolymer was compounded with short carbon fiber (CF) and carbon nanotube (CNT) using a micro-extruder followed by the injection molding process. Composite samples were fabricated with loading ratios of 20 wt.% CF and 0.1, 0.5 and 1.0 wt.% of CNT. Mechanical, electrical, thermo-mechanical, thermal, melt-flow, and structural investigations of ABS-based composites were conducted by performing tensile, impact, hardness, and wear tests, conductive atomic force microscopy (AFM), dynamic mechanical analysis (DMA), thermal gravimetric analysis (TGA), melt flow rate test (MFR), scanning electron microscopy (SEM) characterization techniques, respectively. According to mechanical test data of resultant composites including tensile and impact test findings, CNT additions led to the remarkable increase in tensile strength and impact resistance for CF reinforced ABS composites. The formation of synergy between CNT nanoparticles and CF was confirmed by electrical conduction results. The conductive path in ABS/CF composite system was achieved by the incorporation of CNT with different loading levels. SEM micrographs of composites proved that CNT nanoparticles exhibited homogeneous dispersion into ABS matrix for lower loadings. Graphical abstract: [Figure not available: see fulltext.].Article Citation - WoS: 1Citation - Scopus: 1Gadolinium and Polythiophene Functionalized Polyurea Polymer Dots as Fluoro-Magnetic Nanoprobes(MDPI, 2022) Karabacak, Soner; Palaniappan, Alagappan; Tony, Tsang Siu Hon; Edwin, Teo Hang Tong; Gulyás, Balázs; Padmanabhan, Parasuraman; Yıldız, Ümit HakanA rapid and one-pot synthesis of poly 3-thiopheneacetic acid (PTAA) functionalized pol-yurea polymer dots (Pdots) using polyethyleneimine and isophorone diisocyanate is reported. The one-pot mini-emulsion polymerization technique yielded Pdots with an average diameter of ~20 nm. The size, shape, and concentration of the surface functional groups could be controlled by al-tering the synthesis parameters such as ultrasonication time, concentration of the surfactant, and crosslinking agent, and the types of isocyanates utilized for the synthesis. Colloidal properties of Pdots were characterized using dynamic light scattering and zeta potential measurements. The spherical geometry of Pdots was confirmed by scanning electron microscopy. The Pdots were post-functionalized by 1,4,7,10 tetraazacyclododecane-1,4,7,10-tetraacetic acid for chelating gadolinium nanoparticles (Gd3+) that provide magnetic properties to the Pdots. Thus, the synthesized Pdots possess fluorescent and magnetic properties, imparted by PTAA and Gd3+, respectively. Fluorescence spectroscopy and microscopy revealed that the synthesized dual-functional Gd3+-Pdots ex-hibited detectable fluorescent signals even at lower concentrations. Magnetic levitation experiments indicated that the Gd3+-Pdots could be easily manipulated via an external magnetic field. These findings illustrate that the dua-functional Gd3+-Pdots could be potentially utilized as fluorescent reporters that can be magnetically manipulated for bioimaging applications.Article Citation - WoS: 11Citation - Scopus: 12Colorimetric and Fluorometric Profiling of Advanced Glycation End Products(American Chemical Society, 2022) Ammanath, Gopal; Delachi, Carla Giorgia; Karabacak, Soner; Ali, Yusuf; Boehm, Bernhard O.; Yıldız, Ümit Hakan; Alagappan, Palaniappan; Liedberg, BoProfiling of advanced glycation end products (AGEs) is an emerging area of clinical significance for disease diagnosis and prognosis. Typically, concentrations of AGEs are estimated in laboratories by trained personnel using sophisticated equipment. Herein, a facile approach for colorimetric and fluorometric profiling of AGEs is reported for rapid and on-site analysis. The concentrations of AGE levels in plasma are estimated via changes in optical properties of polythiophenes (PTs) upon interaction with aptamers (Apts) in the presence and in the absence of AGEs. To validate the proposed approach, glyceraldehyde-derived AGEs (AGE class 1 [AGE1]), the biomarker associated with cardiovascular diseases and diabetes, are used as a model system. Colorimetric analysis yielded linear responses for AGE1 for clinically relevant concentration ranges between 1.5 and 300 μg/mL with a limit of detection (LOD) of ∼1.3 μg/mL. Subsequently, an approach utilizing PTs with four different pendant groups in conjunction with four different Apts is demonstrated for qualitative colorimetric profiling and for quantitative fluorometric profiling of up to four AGEs in clinical matrices. Principal component analysis (PCA) of fluorometric responses of AGE-spiked samples yielded distinct responses for the different AGEs tested. Thus, the proposed approach ascertains rapid profiling of spiked AGEs in plasma samples without the requirement of preanalytical processing and advanced instrumentation, thereby facilitating on-site diagnosis.