Scopus İndeksli Yayınlar Koleksiyonu / Scopus Indexed Publications Collection
Permanent URI for this collectionhttps://hdl.handle.net/11147/7148
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Article Synthetic Memory: A Key Link Between Biocatalytically Synthesized Polyesters and Melt Electrowriting Performance(Taylor & Francis inc, 2025) Dinckal, Sanem; Yildiz, Umit HakanThe biocatalytic synthesis of polycaprolactone (PCL) and its copolymers has garnered significant attention due to their reduced toxicity and enhanced 3D processability compared to metal-catalyzed alternatives. The objective of this study is to employ biocatalysts-citric acid (CA), glycolic acid (GA) and salicylic acid (SAA)-and explore their catalytic effects on the synthesis of poly(epsilon-caprolactone) (PCL) and poly(epsilon-caprolactone)-b-poly(delta-valerolactone) (PCL-b-PVL) block copolymers. Additionally, we aimed to examine the link between synthetic memory of resultant PCL and PCL-b-PVL polymers and their melt electrowriting performance. Nuclear magnetic resonance analysis confirms successful synthesis of copolymers by monitoring signals of hydrogens at 2.30 ppm. Differential scanning calorimetry results reveal shifts in thermal properties of copolymers upon varying biocatalysts CA-, SAA- and GA-catalyzed copolymers exhibit Tm values between similar to 52 and 54 degrees C. Melt electrowriting (MEW) results demonstrate that catalyst selection plays significant role in fiber morphology and scaffold architecture, with GA- and CA-catalyzed copolymers exhibiting finer fibers (5-8 mu m), while SAA led to thicker fibers (similar to 12 mu m) and reduced spacing. Moreover, precipitation solvents MeOH and acetonitrile (ACN) affect fidelity, with ACN-prepared scaffolds exhibiting more uniform fiber diameters. Atomic force microscopy imaging of electrowritten scaffolds made of ACN- and MeOH-precipitated PCL-b-PVL both exhibit large (>15 mu m) and smaller (<10 mu m) spherulitic structure as major topological features. These findings confirm that the synthetic memory of polyesters-governed by catalyst choice and processing conditions-directly influences their printability, making them promising candidates for MEW-based biomedical scaffolds in tissue engineering, where fine fiber morphology and architectural fidelity are essential for cell attachment and tissue regeneration.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.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: 40Citation - Scopus: 41Colorimetric Urinalysis for On-Site Detection of Metabolic Biomarkers(American Chemical Society, 2020) Yeasmin, Sanjida; Ammanath, Gopal; Ali, Yusuf; Boehm, Bernhard O.; Yıldız, Ümit Hakan; Palaniappan, Alagappan; Liedberg, BoOver the past few decades, colorimetric assays have been developed for cost-effective and rapid on-site urinalysis. Most of these assays were employed for detection of biomarkers such as glucose, uric acid, ions, and albumin that are abundant in urine at micromolar to millimolar levels. In contrast, direct assaying of urinary biomarkers such as glycated proteins, low-molecular-weight reactive oxygen species, and nucleic acids that are present at significantly lower levels (nanomolar to picomolar) remain challenging due to the interferences from the urine sample matrix. State-of-the-art assays for detection of trace amounts of urinary biomarkers typically utilize time-consuming and equipment-dependent sample pretreatment or clean-up protocols prior to assaying, which limits their applicability for on-site analysis. Herein, we report a colorimetric assay for on-site detection of trace amount of generic biomarkers in urine without involving tedious sample pretreatment protocols. The detection strategy is based on monitoring the changes in optical properties of poly(3-(4-methyl-3'-thienyloxy)propyltriethylammonium bromide) upon interacting with an aptamer or a peptide nucleic acid in the presence and absence of target biomarkers of relevance for the diagnosis of metabolic complications and diabetes. As a proof of concept, this study demonstrates facile assaying of advanced glycation end products, 8-hydroxy-2'-deoxyguanosine and hepatitis B virus DNA in urine samples at clinically relevant concentrations, with limits of detection of similar to 850 pM, similar to 650 pM, and similar to 1 nM, respectively. These analytes represent three distinct classes of biomarkers: (i) glycated proteins, (ii) low-molecular-weight reactive oxygen species, and (iii) nucleic acids. Hence, the proposed methodology is applicable for rapid detection of generic biomarkers in urine, without involving sophisticated equipment and skilled personnel, thereby enabling on-site urinalysis. At the end of the contribution, we discuss the opportunity to translate the homogeneous assay into a paper-based format.Article Citation - WoS: 6Citation - Scopus: 8Outer-Membrane Protease (ompt) Based E.coli Sensing With Anionic Polythiophene and Unlabeled Peptide Substrate(John Wiley and Sons Inc., 2020) Sinsinbar, Gaurav; Gudlur, Sushanth; Wood, Sarah E.; Ammanath, Gopal; Yıldız, Ümit Hakan; Alagappan, Palaniappan; Liedberg, BoE. coli and Salmonella are two of the most common bacterial pathogens involved in foodborne and waterborne related deaths. Hence, it is critical to develop rapid and sensitive detection strategies for near-outbreak applications. Reported is a simple and specific assay to detect as low as 1 CFU mL(-1)of E. coli in water within 6 hours by targeting the bacteria's surface protease activity. The assay relies on polythiophene acetic acid (PTAA) as an optical reporter and a short unlabeled peptide (LL37(FRRV)) previously optimized as a substrate for OmpT, an outer-membrane protease on E. coli. LL37(FRRV)interacts with PTAA to enhance its fluorescence while also inducing the formation of a helical PTAA-LL37(FRRV)construct, as confirmed by circular dichroism. However, in the presence of E. coli LL37(FRRV)is cleaved and can no longer affect the conformations and optical properties of PTAA. This ability to distinguish between an intact and cleaved peptide was investigated in detail using LL37(FRRV)sequence variants.Article Citation - WoS: 27Citation - Scopus: 28Biocomposite Scaffolds for 3d Cell Culture: Propolis Enriched Polyvinyl Alcohol Nanofibers Favoring Cell Adhesion(John Wiley and Sons Inc., 2021) Bilginer, Rumeysa; Özkendir İnanç, Dilce; Yıldız, Ümit Hakan; Arslan Yıldız, AhuThe objective of this work is generation of propolis/polyvinyl alcohol (PVA) scaffold by electrospinning for 3D cell culture. Here, PVA used as co-spinning agent since propolis alone cannot be easily processed by electrospinning methodology. Propolis takes charge in maximizing biological aspect of scaffold to facilitate cell attachment and proliferation. Morphological analysis showed size of the electrospun nanofibers varied between 172-523 nm and 345-687 nm in diameter, for non-crosslinked and crosslinked scaffolds, respectively. Incorporation of propolis resulted in desired surface properties of hybrid matrix, where hybrid scaffolds highly favored protein adsorption. To examine cell compatibility, NIH-3T3 and HeLa cells were seeded on propolis/PVA hybrid scaffold. Results confirmed that integration of propolis supported cell adhesion and cell proliferation. Also, results indicated electrospun propolis/PVA hybrid scaffold provide suitable microenvironment for cell culturing. Therefore, developed hybrid scaffold could be considered as potential candidate for 3D cell culture and tissue engineering.Article Citation - WoS: 5Citation - Scopus: 6Boosting Up Printability of Biomacromolecule Based Bio-Ink by Modulation of Hydrogen Bonding Pairs(Elsevier Ltd., 2020) Köksal, Büşra; Önbaş, Rabia; Başkurt, Mehmet; Şahin, Hasan; Arslan Yıldız, Ahu; Yıldız, Ümit HakanThis study describes low dose UV curable and bioprintable new bioink made of hydrogen bond donor-acceptor adaptor molecule 2-isocyanatoethyl methacrylate (NCO)modified gelatin (NCO-Gel). Our theoretical calculations demonstrate that insertion of 2-isocyanatoethyl methacrylate doubles the interaction energy (500 meV) between gelatin chains providing significant contribution in interchain condensation and self-organization as compared to methacrylic anhydride modified gelatin (GelMA). The NCO-Gel exhibits peak around 1720 cm?1 referring to bidentate hydrogen bonding between H-NCO and its counterpart O[dbnd]CN[sbnd]H. These strong interchain interactions drive chains to be packed and thereby facilitating UV crosslinking. The NCO-Gel is exhibiting a rapid, 10 s gelation process by the exposure of laser (3 W, 365 nm). The dynamic light scattering characterization also reveals that NCO-Gel has faster sol to gel transition as compared to GelMA depending on the UV curing time. The NCO-Gel was found to be more firm and mechanically strong that provides advantages in molding as well as bioprinting processes. Bioprinted NCO-Gel has shown sharp borders and stable 3D geometry as compared to GelMA ink under 10 s UV curing time. The cell viability tests confirm that NCO-Gel facilitates cell proliferation and supports cell viability. We foresee that NCO-Gel bioink formulation provides a promising opportunity when low dose UV curing and rapid printing are required. © 2020 Elsevier LtdArticle Citation - WoS: 3Citation - Scopus: 4Lipid Bilayer on Wrinkled-Interfaced Graphene Field Effect Transistor(Elsevier Ltd., 2021) Özkendir İnanç, Dilce; Çelebi, Cem; Yıldız, Ümit HakanThis study describes lipid bilayer-based sensor interface on SiO2 encapsulated graphene field effect transistors (GFET). The SiO2 layer was utilized as a lipid compatible surface that drives bilayer formation. The two types of surface morphologies i) wrinkled morphology by thermal evaporation (TE) and ii) flat morphology by pulsed electron deposition (PED) were obtained. The sensing performance of wrinkled and flat interfaced-GFETs were investigated, pH sensitivity of wrinkled interfaced-GFETs were found to be ten fold larger than the flat ones. The enhanced sensitivity is attributed to thinning of the oxide layer by formation of wrinkles thereby facilitating electrostatic gating on graphene. We foresee that described wrinkled SiO2 interfaced-GFET holds promise as a cell membrane mimicking sensing platform for novel bioelectronic applications. © 2020