Dataset Information

Electrochemical Redox Refrigeration.

ABSTRACT: The high conformational entropy change of the Fe(CN)63-/4- redox reaction can be used as the basis for a compact electrochemical refrigerator. This device is comparable to a liquid version of a Peltier cooler, with two distinct advantages: (1) the entropy change per carrier (1.5?mV/K) of the electrochemical refrigerant is more than 5 times larger than that of state-of-the-art solid thermoelectric materials; and (2) the liquid electrolyte can be advected continuously away from the cooling junction, so that Joule heating in the bulk element does not diminish the delivered cooling effect. In this work, we use infrared microscopy to visualize the thermal aspects of Fe(CN)63-/4- redox, and compare the estimated cooling to calculated values with and without electrolyte flow. While the temperature differences achieved in a single cell are small (~50?mK) and not enhanced by electrolyte flow, the cooling power density (~0.5?W/cm3) is high when normalized to the small electrode volume. Non-dimensional figures of merit are proposed to identify electrochemical redox species for maximizing the cooling effect.

SUBMITTER: McKay IS

PROVIDER: S-EPMC6763465 | biostudies-literature | 2019 Sep

REPOSITORIES: biostudies-literature

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Electrochemical Redox Refrigeration.

McKay Ian S IS Kunz Larissa Y LY Majumdar Arun A

Scientific reports 20190926 1

The high conformational entropy change of the Fe(CN)<sub>6</sub><sup>3-/4-</sup> redox reaction can be used as the basis for a compact electrochemical refrigerator. This device is comparable to a liquid version of a Peltier cooler, with two distinct advantages: (1) the entropy change per carrier (1.5 mV/K) of the electrochemical refrigerant is more than 5 times larger than that of state-of-the-art solid thermoelectric materials; and (2) the liquid electrolyte can be advected continuously away fr ...[more]

PMID: 31558735

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Project description:Recent years have seen the development of a large number of electrochemical sandwich assays and reagentless biosensor architectures employing biomolecules modified via the attachment of a redox-active "reporter." Here we survey a large set of potential redox reporters in order to determine which exhibits the best long-duration stability in thiol-on-gold monolayer-based sensors and to identify reporter "sets" signaling at distinct, nonoverlapping redox potentials in support of multiplexing and error correcting ratiometric or differential measurement approaches. Specifically, we have characterized the performance of more than a dozen potential reporters that are, first, redox active within the potential window over which thiol-on-gold monolayers are reasonably stable and, second, are available commercially in forms that are readily conjugated to biomolecules or can be converted into such forms in one or two simple synthetic steps. To test each of these reporters we conjugated it to one terminus of a single-stranded DNA "probe" that was attached by its other terminus via a six-carbon thiol to a gold electrode to form an "E-DNA" sensor responsive to its complementary DNA target. We then measured the signaling properties of each sensor as well as its stability against repeated voltammetric scans and against deployment in and reuse from blood serum. Doing so we find that the performance of methylene blue-based, thiol-on-gold sensors is unmatched; the near-quantitative stability of such sensors against repeated scanning in even very complex sample matrices is unparalleled. While more modest, the stability of sensors employing a handful of other reporters, including anthraquinone, Nile blue, and ferrrocene, is reasonable. Our work thus serves as both to highlight the exceptional properties of methylene blue as a redox reporter in such applications and as a cautionary tale-we wish to help other researchers avoid fruitless efforts to employ the many, seemingly promising and yet ultimately inadequate reporters we have investigated. Finally, we hope that our work also serves as an illustration of the pressing need for the further development of useful redox reporters.

Dataset Information

Electrochemical Redox Refrigeration.

Publications

Electrochemical Redox Refrigeration.

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