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Abstract Redox, a native modality in biology involving the flow of electrons, energy, and information, is used for energy‐harvesting, biosynthesis, immune‐defense, and signaling. Because electrons (in contrast to protons) are not soluble in the medium, electron‐flow through the redox modality occurs through redox reactions that are sometimes organized into pathways and networks (e.g., redox interactomes). Redox is also accessible to electrochemistry, which enables electrodes to receive and transmit electrons to exchange energy and information with biology. In this Perspective, efforts to develop electrochemistry as a tool for redox‐based bio‐information processing: to interconvert redox‐based molecular attributes into interpretable electronic signals, are described. Using a series of Case Studies, how the information‐content of the measurements can be enriched using: diffusible mediators; tuned electrical input sequences; and cross‐modal measurements (e.g., electrical plus spectral), is shown. Also, theory‐guided feature engineering approaches to compress the information in the electronic signals into quantitative metrics (i.e., features) that can serve as correlating variables for pattern recognition by data‐driven analysis are described. Finally, how redox provides a modality for electrogenetic actuation is illustrated. It is suggested that electrochemistry's capabilities to provide real‐time, low‐cost, and high‐content data in an electronic format allow the feedback‐control needed for autonomous learning and deployable sensing/actuation. 

Abstract We report the integration of 3D printing, electrobiofabrication, and protein engineering to create a device that enables near real‐time analysis of monoclonal antibody (mAb) titer and quality. 3D printing was used to create the macroscale architecture that can control fluidic contact of a sample with multiple electrodes for replicate measurements. An analysis “chip” was configured as a “snap‐in” module for connecting to a 3D printed housing containing fluidic and electronic communication systems. Electrobiofabrication was used to functionalize each electrode by the assembly of a hydrogel interface containing biomolecular recognition and capture proteins. Specifically, an electrochemical thiol oxidation is used to assemble a thiolated polyethylene glycol hydrogel, that in turn is covalently coupled to either a cysteine‐tagged protein G that binds the antibody's Fc region or a lectin that binds the glycans of target mAb analytes. We first show the design, assembly, and testing of the hardware device. Then, we show the transition of a step‐by‐step sensing methodology (e.g., mix, incubate, wash, mix, incubate, wash, measure) into the current method where functionalization, antibody capture, and assessment are performed in situ and in parallel channels. Both titer and glycan analyses were found to be linear with antibody concentration (to 0.2 mg/L). We further found the interfaces could be reused with remarkably similar results. Because the interface assembly and use are simple, rapid, and robust, we suggest this assessment methodology will be widely applicable, including for other biomolecular process development and manufacturing environments. 

Melanins have complex structures, difficult-to-characterize properties, and poorly understood biological functions. Electrochemical methods are revealing how melanin's redox-state molecular-switching is coupled to its electron-transfer activities.