A novel electrochemical dopamine sensor was fabricated based on a composite film solely consisting of kappa-carrageenan and hierarchical porous carbon drop-casted onto a glassy carbon electrode in a conventional three electrode system. Graphene oxide was synthesized in a one-step thermal conversion from base-catalyzed alkali lignin. Five ratios by mass of a novel hierarchical porous activated carbon and kappa-carrageenan were studied for dopamine quantification without synthetic binders such as polytetrafluoroethylene. Various tests were performed to explicate structure and electrochemical properties of the films. Utilizing differential pulse voltammetry for detection, the optimized 10:1 ratio system elicited a linear range of 1–250
- Award ID(s):
- 1933861
- NSF-PAR ID:
- 10297912
- Date Published:
- Journal Name:
- RSC Advances
- Volume:
- 11
- Issue:
- 25
- ISSN:
- 2046-2069
- Page Range / eLocation ID:
- 15410 to 15415
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
more » « less
μ mol l−1and a limit of detection of 0.14μ mol l−1(S/N = 3). Results suggested an effective new combination of materials for non-enzymatic dopamine sensing. -
Measurements of the gas sensing performance of nanomaterials typically involve the use of interdigitated electrodes (IDEs). A separate heater is often integrated to provide elevated temperature for improved sensing performance. However, the use of IDEs and separate heaters increases fabrication complexity. Here, a novel gas sensing platform based on a highly porous laser-induced graphene (LIG) pattern is reported. The LIG gas sensing platform consists of a sensing region and a serpentine interconnect region. A thin film of metal ( e.g. , Ag) coated in the serpentine interconnect region significantly reduces its resistance, thereby providing a localized Joule healing in the sensing region ( i.e. , self-heating) during typical measurements of chemoresistive gas sensors. Dispersing nanomaterials with different selectivity in the sensing region results in an array to potentially deconvolute various gaseous components in the mixture. The self-heating of the LIG gas sensing platform is first studied as a function of the applied voltage during resistance measurement and LIG geometric parameters ( e.g. , linewidth from 120 to 240 μm) to achieve an operating temperature from 20 to 80 °C. Systematic investigations of various nanomaterials demonstrate the feasibility of the LIG gas sensing performance. Taken together with the stretchable design layout in the serpentine interconnect region to provide mechanical robustness over a tensile strain of 20%, the gas sensor with a significant response (6.6‰ ppm −1 ), fast response/recovery processes, excellent selectivity, and an ultralow limit of detection (1.5 parts per billion) at a modest temperature from self-heating opens new opportunities in epidermal electronic devices.more » « less
-
more » « less
Neurotransmitters are small molecules involved in neuronal signaling and can also serve as stress biomarkers.1Their abnormal levels have been also proposed to be indicative of several neurological diseases such as Alzheimer’s disease, Parkinson’s disease, Huntington disease, among others. Hence, measuring their levels is highly important for early diagnosis, therapy, and disease prognosis. In this work, we investigate facile functionalization methods to tune and enhance sensitivity of printed graphene sensors to neurotransmitters. Sensors based on direct laser scribing and screen-printed graphene ink are studied. These printing methods offer ease of prototyping and scalable fabrication at low cost.
The effect of functionalization of laser induced graphene (LIG) by electrodeposition and solution-based deposition of TMDs (molybdenum disulfide2and tungsten disulfide) and metal nanoparticles is studied. For different processing methods, electrochemical characteristics (such as electrochemically active surface area: ECSA and heterogenous electron transfer rate: k0) are extracted and correlated to surface chemistry and defect density obtained respectively using X-ray photoelectron spectroscopy (XPS) and Raman spectroscopy. These functionalization methods are observed to directly impact the sensitivity and limit of detection (LOD) of the graphene sensors for the studied neurotransmitters. For example, as compared to bare LIG, it is observed that electrodeposition of MoS2on LIG improves ECSA by 3 times and k0by 1.5 times.3Electrodeposition of MoS2also significantly reduces LOD of serotonin and dopamine in saliva, enabling detection of their physiologically relevant concentrations (in pM-nM range). In addition, chemical treatment of LIG sensors is carried out in the form of acetic acid treatment. Acetic acid treatment has been shown previously to improve C-C bonds improving the conductivity of LIG sensors.4In our work, in particular, acetic acid treatment leads to larger improvement of LOD of norepinephrine compared to MoS2electrodeposition.
In addition, we investigate the effect of plasma treatment to tune the sensor response by modifying the defect density and chemistry. For example, we find that oxygen plasma treatment of screen-printed graphene ink greatly improves LOD of norepinephrine up to three orders of magnitude, which may be attributed to the increased defects and oxygen functional groups on the surface as evident by XPS measurements. Defects are known to play a key role in enhancing the sensitivity of 2D materials to surface interactions, and have been explored in tuning/enhancing the sensor sensitivity.5Building on our previous work,3we apply a custom machine learning-based data processing method to further improve that sensitivity and LOD, and also to automatically benchmark different molecule-material pairs.
Future work includes expanding the plasma chemistry and conditions, studying the effect of precursor mixture in laser-induced solution-based functionalization, and understanding the interplay between molecule-material system. Work is also underway to improve the machine learning model by using nonlinear learning models such as neural networks to improve the sensor sensitivity, selectivity, and robustness.
References A. J. Steckl, P. Ray, (2018), doi:10.1021/acssensors.8b00726.
Y. Lei, D. Butler, M. C. Lucking, F. Zhang, T. Xia, K. Fujisawa, T. Granzier-Nakajima, R. Cruz-Silva, M. Endo, H. Terrones, M. Terrones, A. Ebrahimi,
Sci. Adv. 6 , 4250–4257 (2020).V. Kammarchedu, D. Butler, A. Ebrahimi,
Anal. Chim. Acta .1232 , 340447 (2022).H. Yoon, J. Nah, H. Kim, S. Ko, M. Sharifuzzaman, S. C. Barman, X. Xuan, J. Kim, J. Y. Park,
Sensors Actuators B Chem. 311 , 127866 (2020).T. Wu, A. Alharbi, R. Kiani, D. Shahrjerdi,
Adv. Mater. 31 , 1–12 (2019). -
This study aimed to explore lignin as a naturally occurring aromatic precursor for the synthesis of LIG and further fabrication of ultrasensitive strain sensors for the detection of small deformations. One-step direct laser writing (DLW) induced high quality porous graphene, so called laser induced graphene (LIG), from kraft lignin under the conditions optimized for laser power, focus distance, and lignin loading. An electrode based on the resulting LIG was facilely fabricated by transferring LIG onto an elastomeric substrate ( i.e. , Dragon Skin™). The novel LIG transfer was facilitated by spin coating followed by water lifting, leading to the full retention of porous graphene onto the elastomeric substrate. The strain sensor was shown to be highly sensitive to small human body motions and tiny deformations caused by vibrations. It had a working range of up to 14% strain with a gauge factor of 960 and showed high stability as evidenced by repetitive signals over 10 000 cycles at 4% strain. The sensor was also successfully demonstrated for detecting human speaking, breath, seismocardiography (SCG), and movement of pulse and eye. Overall, the lignin-derived LIG can serve as excellent piezoresistive materials for wearable, stretchable, and ultrasensitive strain sensors with applications in human body motion monitoring and sound-related applications.more » « less
-
more » « less
Pseudomonas aeruginosa (P. aeruginosa ) is a phenazine-producing pathogen recognized for its biofilm-mediated antibiotic resistance, showing up to 1000 times higher resistance compared to planktonic cells. In particular, it is shown that a phenazine called pyocyanin promotes antibiotic tolerance inP. aeruginosa cultures by upregulating efflux pumps and inducing biofilm formation. Therefore, real-time study of phenazine production in response to antibiotics could offer new insights for early detection and management of the infection. Toward this goal, this work demonstrates real-time monitoring ofP. aeruginosa colony biofilms challenged by antibiotics using electrochemical sensors based on direct laser functionalization of laser induced graphene (LIG) with gold (Au) nanostructures. Specifically, two routes for functionalization of the LIG electrodes with Au-containing solutions are studied: electroless deposition and direct laser functionalization (E-Au/LIG and L-Au/LIG, respectively). While both methods show comparable sensitivity (1.276 vs 1.205μ Aμ M−1), E-Au/LIG has bactericidal effects which make it unsuitable as a sensor material. The effect of antibiotics (gentamicin as a model drug) on the production rate of phenazines before (i.e., in planktonic phase) or after biofilm formation is studied. The sensor data confirms that theP. aeruginosa biofilms are at least 100 times more tolerant to the antibiotic compared to planktonic cells. The biosensors are developed using a scalable and facile manufacturing approach and may pave the way toward simple-to-use antibiotic susceptibility testing devices for early infection diagnosis and real-time study of antibiotic resistance evolution.
- Free Publicly Accessible Full Text
-
Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1039/D1RA00735A
