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Reversible Interconversion of CO<sub>2</sub> and Formate by a Molybdenum-Containing Formate Dehydrogenase
CO<sub>2</sub> and formate are rapidly, selectively, and efficiently
interconverted by tungsten-containing formate dehydrogenases that
surpass current synthetic catalysts. However, their mechanism of catalysis
is unknown, and no tractable system is available for study. Here,
we describe the catalytic properties of the molybdenum-containing
formate dehydrogenase H from the model organism Escherichia
coli (<i>Ec</i>FDH-H). We use protein film
voltammetry to demonstrate that <i>Ec</i>FDH-H is a highly
active, reversible electrocatalyst. In each voltammogram a single
point of zero net current denotes the CO<sub>2</sub> reduction potential
that varies with pH according to the Nernst equation. By quantifying
formate production we show that electrocatalytic CO<sub>2</sub> reduction
is specific. Our results reveal the capabilities of a Mo-containing
catalyst for reversible CO<sub>2</sub> reduction and establish <i>Ec</i>FDH-H as an attractive model system for mechanistic investigations
and a template for the development of synthetic catalysts
Engineering a Point-of-Care Paper-Microfluidic Electrochemical Device Applied to the Multiplexed Quantitative Detection of Biomarkers in Sputum
Health initiatives worldwide demand affordable point-of-care
devices
to aid in the reduction of morbidity and mortality rates of high-incidence
infectious and noncommunicable diseases. However, the production of
robust and reliable easy-to-use diagnostic platforms showing the ability
to quantitatively measure several biomarkers in physiological fluids
and that could in turn be decentralized to reach any relevant environment
remains a challenge. Here, we show the particular combination of paper-microfluidic
technology, electrochemical transduction, and magnetic nanoparticle-based
immunoassay approaches to produce a unique, compact, and easily deployable
multiplex device to simultaneously measure interleukin-8, tumor necrosis
factor-α, and myeloperoxidase biomarkers in sputum, developed
with the aim of facilitating the timely detection of acute exacerbations
of chronic obstructive pulmonary disease. The device incorporates
an on-chip electrochemical cell array and a multichannel paper component,
engineered to be easily aligned into a polymeric cartridge and exchanged
if necessary. Calibration curves at clinically relevant biomarker
concentration ranges are produced in buffer and artificial sputum.
The analysis of sputum samples of healthy individuals and acutely
exacerbated patients produces statistically significant biomarker
concentration differences between the two studied groups. The device
can be mass-produced at a low cost, being an easily adaptable platform
for measuring other disease-related target biomarkers