期刊名称：Proceedings of the National Academy of Sciences
印刷版ISSN：0027-8424
电子版ISSN：1091-6490
出版年度：2016
卷号：113
期号：51
页码：14633-14638
DOI：10.1073/pnas.1625010114
语种：English
出版社：The National Academy of Sciences of the United States of America
摘要：SignificanceNanoelectronic transistor sensors based on synthesized one- and two-dimensional nanomaterials have achieved real-time label-free detection of a wide range of biological species with high sensitivity, although direct analysis of biological samples has been limited due to Debye charge screening in physiological solutions. This paper describes a general strategy overcoming this challenge involving comodification of the transistor sensor surface with a polymer and receptor, where the polymer forms a permeable layer that increases the effective screening length and receptor enables selective detection of analytes. The capability of this strategy was demonstrated with selective detection of cancer markers in physiological solution, thus opening substantial opportunities for real-time sensing applications in biology and medicine. Nanomaterial-based field-effect transistor (FET) sensors are capable of label-free real-time chemical and biological detection with high sensitivity and spatial resolution, although direct measurements in high-ionic-strength physiological solutions remain challenging due to the Debye screening effect. Recently, we demonstrated a general strategy to overcome this challenge by incorporating a biomolecule-permeable polymer layer on the surface of silicon nanowire FET sensors. The permeable polymer layer can increase the effective screening length immediately adjacent to the device surface and thereby enable real-time detection of biomolecules in high-ionic-strength solutions. Here, we describe studies demonstrating both the generality of this concept and application to specific protein detection using graphene FET sensors. Concentration-dependent measurements made with polyethylene glycol (PEG)-modified graphene devices exhibited real-time reversible detection of prostate specific antigen (PSA) from 1 to 1,000 nM in 100 mM phosphate buffer. In addition, comodification of graphene devices with PEG and DNA aptamers yielded specific irreversible binding and detection of PSA in pH 7.4 1x PBS solutions, whereas control experiments with proteins that do not bind to the aptamer showed smaller reversible signals. In addition, the active aptamer receptor of the modified graphene devices could be regenerated to yield multiuse selective PSA sensing under physiological conditions. The current work presents an important concept toward the application of nanomaterial-based FET sensors for biochemical sensing in physiological environments and thus could lead to powerful tools for basic research and healthcare.
