TY - JOUR
T1 - Improving the sensitivity of electrochemical sensors through a complementary luminescent mode
T2 - A new spectroelectrochemical approach
AU - Chatterjee, Sayandev
AU - Fujimoto, Meghan S.
AU - Cheng, Yu Hsuan
AU - Kargupta, Roli
AU - Soltis, Jennifer A.
AU - Motkuri, Radha Kishan
AU - Basuray, Sagnik
N1 - Funding Information:
This research was supported by (1) the Laboratory Directed Research and Development Program at the Pacific Northwest National Laboratory (SEED EED) (S.C.) and (2) a National Science Foundation (NSF) Career grant (#1751759 ), "ASSURED electrochemical platform for multiplexed detection of Cancer Biomarker Panel using Shear-Enhanced Nanoporous-Capacitive Electrodes” (S.B.). Pacific Northwest National Laboratory (PNNL) is operated by Battelle for the U.S. Department of Energy under Contract DE-AC05-76RL01830. We would like to especially acknowledge Dr. Tatiana Levitskaia for helpful discussions. Part of this research was performed at Environmental Molecular Sciences Laboratory, a national scientific user facility at PNNL managed by the Department of Energy’s Office of Biological and Environmental Research.
Publisher Copyright:
© 2018 Elsevier B.V.
PY - 2019/4/1
Y1 - 2019/4/1
N2 - Rapid and sensitive detection and quantification of trace and ultra-trace analytes is critical to environmental remediation, analytical chemistry and defense from chemical and biological contaminants. Though affinity based electrochemical sensors have gained immense popularity, they frequently do not meet the requirements of desired sensitivity and detection limits. Here, we demonstrate a complementary luminescence mode that can significantly enhance sensitivity of impedance or voltammetric electrochemical sensors. Our methodology involves using a redox probe, whose luminescence properties change upon changing the oxidation state. By tailoring the system such that these luminescence changes can be correlated with the capture of target analytes, we are able to significantly lower the detection limit and improve the efficiency of detection compared to the electrochemical modes alone. Our proof-of-concept demonstration, using a model system designed for Ca2+ capture, illustrated that the luminescent mode allowed us to lower the limits of detection by three-orders of magnitude compared to the impedance or voltammetric modes alone without requiring any modification of electrode design or cell configuration. Further, the linear ranges of detection are 10−8 to 10−3 M in the voltammetry mode, 10−8 to 10−5 M in the impedance mode and 2.5 × 10−11 to 10−7 M in the luminescent mode, providing a large range of operational flexibility.
AB - Rapid and sensitive detection and quantification of trace and ultra-trace analytes is critical to environmental remediation, analytical chemistry and defense from chemical and biological contaminants. Though affinity based electrochemical sensors have gained immense popularity, they frequently do not meet the requirements of desired sensitivity and detection limits. Here, we demonstrate a complementary luminescence mode that can significantly enhance sensitivity of impedance or voltammetric electrochemical sensors. Our methodology involves using a redox probe, whose luminescence properties change upon changing the oxidation state. By tailoring the system such that these luminescence changes can be correlated with the capture of target analytes, we are able to significantly lower the detection limit and improve the efficiency of detection compared to the electrochemical modes alone. Our proof-of-concept demonstration, using a model system designed for Ca2+ capture, illustrated that the luminescent mode allowed us to lower the limits of detection by three-orders of magnitude compared to the impedance or voltammetric modes alone without requiring any modification of electrode design or cell configuration. Further, the linear ranges of detection are 10−8 to 10−3 M in the voltammetry mode, 10−8 to 10−5 M in the impedance mode and 2.5 × 10−11 to 10−7 M in the luminescent mode, providing a large range of operational flexibility.
KW - Affinity sensors
KW - Limit of detection
KW - Luminescent sensors
KW - Rapid detection
KW - Sensitivity enhancement
KW - Spectroelectrochemistry
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U2 - 10.1016/j.snb.2018.10.093
DO - 10.1016/j.snb.2018.10.093
M3 - Article
AN - SCOPUS:85059684612
SN - 0925-4005
VL - 284
SP - 663
EP - 674
JO - Sensors and Actuators, B: Chemical
JF - Sensors and Actuators, B: Chemical
ER -