Telma Domingues, Chun-Da Liao, Marta Prado, M. Fátima Cerqueira, Dmitri Y. Petrovykh, Pedro Alpuim, Jérôme Borme, Joana Rafaela Guerreiro
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引用次数: 0
Abstract
This study investigates the effect of different linkers and solvents on the immobilization of DNA probes on graphene surfaces, which are crucial for developing high-performance biosensors. Quartz crystal microbalance with dissipation (QCM-D) measurements were used to characterize in situ and real-time the immobilization of ssDNA and hybridization efficiency on model graphene surfaces. The DNA probes immobilization kinetics and thermodynamics were systematically investigated for all the pairings between three bifunctional linkers─1-pyrenebutyric acid succinimidyl ester (PBSE), Fluorenylmethylsuccinimidyl carbonate (FSC), and Acridine Orange (AO) succinimidyl ester─and three organic solvents (DMF, DMSO, and 10% DMF/ethanol). The linker’s spatial orientation and effective surface modification for DNA probe attachment were also evaluated based on footprints and DNA probe surface coverage. Graphene surfaces functionalized with PBSE in DMF achieved the highest DNA probe surface density (up to 1.31 × 1013 molecules cm–2) and fastest kinetic, p values above 4, and hybridization efficiencies of at least 70%, with 20 to 30% of ssDNA directly adsorbed nonspecifically on the functionalized graphene surface, which has significant implications for the design of sensitive biosensors. The efficiency of the ethanolamine-NHS blocking reaction was estimated to be 80%. The surface packing density of the linker was estimated at 25% of the entire surface coverage for PBSE, and about 22 and 13% for AO and FSC, respectively. Overall, the surface coverage achieved for probe DNA was in the same order of magnitude as that obtained on flat gold surfaces (≥1013 molecules cm–2), typically used in biosensors. These findings highlight the importance of the selected conditions for graphene surface modification to achieve high DNA probe surface density on graphene materials. These results underscore the critical role of interface engineering in achieving target functional outcomes in biosensing technology.
期刊介绍:
Langmuir is an interdisciplinary journal publishing articles in the following subject categories:
Colloids: surfactants and self-assembly, dispersions, emulsions, foams
Interfaces: adsorption, reactions, films, forces
Biological Interfaces: biocolloids, biomolecular and biomimetic materials
Materials: nano- and mesostructured materials, polymers, gels, liquid crystals
Electrochemistry: interfacial charge transfer, charge transport, electrocatalysis, electrokinetic phenomena, bioelectrochemistry
Devices and Applications: sensors, fluidics, patterning, catalysis, photonic crystals
However, when high-impact, original work is submitted that does not fit within the above categories, decisions to accept or decline such papers will be based on one criteria: What Would Irving Do?
Langmuir ranks #2 in citations out of 136 journals in the category of Physical Chemistry with 113,157 total citations. The journal received an Impact Factor of 4.384*.
This journal is also indexed in the categories of Materials Science (ranked #1) and Multidisciplinary Chemistry (ranked #5).