title: Electrochemical Probing through a Redox Capacitor To Acquire Chemical Information on Biothiols.
abstract: The acquisition of chemical information is a critical need for medical diagnostics, food/environmental monitoring, and national security. Here, we report an electrochemical information processing approach that integrates (i) complex electrical inputs/outputs, (ii) mediators to transduce the electrical I/O into redox signals that can actively probe the chemical environment, and (iii) a redox capacitor that manipulates signals for information extraction. We demonstrate the capabilities of this chemical information processing strategy using biothiols because of the emerging importance of these molecules in medicine and because their distinct chemical properties allow evaluation of hypothesis-driven information probing. We show that input sequences can be tailored to probe for chemical information both qualitatively (step inputs probe for thiol-specific signatures) and quantitatively. Specifically, we observed picomolar limits of detection and linear responses to concentrations over 5 orders of magnitude (1 pM-0.1 μM). This approach allows the capabilities of signal processing to be extended for rapid, robust, and on-site analysis of chemical information.
authors.affiliation: Department of Biomedical Engineering, School of Geosciences and Info-Physics, Central South University , Changsha 410083, People's Republic of China.|Institute for Bioscience and Biotechnology Research and Fischell Department of Bioengineering, University of Maryland , College Park, Maryland 20742, United States.
authors.forename: Zhengchun
authors.initials: Z
authors.lastname: Liu
authors.affiliation: Institute for Bioscience and Biotechnology Research and Fischell Department of Bioengineering, University of Maryland , College Park, Maryland 20742, United States.
authors.forename: Yi
authors.initials: Y
authors.lastname: Liu
authors.affiliation: Institute for Bioscience and Biotechnology Research and Fischell Department of Bioengineering, University of Maryland , College Park, Maryland 20742, United States.
authors.forename: Eunkyoung
authors.initials: E
authors.lastname: Kim
authors.affiliation: Institute for Bioscience and Biotechnology Research and Fischell Department of Bioengineering, University of Maryland , College Park, Maryland 20742, United States.
authors.forename: William E
authors.initials: WE
authors.lastname: Bentley
authors.affiliation: Institute for Bioscience and Biotechnology Research and Fischell Department of Bioengineering, University of Maryland , College Park, Maryland 20742, United States.
authors.forename: Gregory F
authors.initials: GF
authors.lastname: Payne
mesh_terms: D002396:Catechols / Q000737:chemistry; D048271:Chitosan / Q000737:chemistry; D056831:Coordination Complexes / Q000737:chemistry; D003545:Cysteine / Q000032:analysis; D055664:Electrochemical Techniques / Q000379:methods*; D004566:Electrodes; D005978:Glutathione / Q000737:chemistry; D006046:Gold / Q000737:chemistry; D010084:Oxidation-Reduction; D056951:Photoelectron Spectroscopy; D013438:Sulfhydryl Compounds / Q000032:analysis*
chemical_list: D002396:Catechols; D056831:Coordination Complexes; D013438:Sulfhydryl Compounds; D006046:Gold; D048271:Chitosan; D005978:Glutathione; D003545:Cysteine; C034221:catechol