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Enzymatic self-wiring in nanopores and its application in direct electron transfer biofuel cells.

ABSTRACT: A synthetic enzymatic activity in nanopores leading to the direct fabrication of modified electrodes applicable as biosensors and/or biofuel cell elements is reported. We demonstrate the heterogeneous enzymatic implanting of platinum nanoclusters, PtNCs, in glucose oxidase, GOx, immobilized on mesoporous carbon nanoparticles, MPCNP-modified surface. As the pores confine the growth of the clusters, the PtNC@GOx/MPCNP assembly becomes electrically wired to the matrix, demonstrating direct electron transfer, DET, bioelectrocatalytic properties that correlate with the applied duration of synthesis and cluster size. This inside-out nanocluster growth from the cofactor to the matrix is investigated and further compared to a reversed outside-in strategy which follows the electrochemical deposition of the Pt clusters inside the pores and their electrically induced expansion towards the FAD center of the enzyme. While the inside-out and outside-in methodologies provide, for the first time, synthetic bidirectional direct wiring routes of an enzyme to a surface, we highlight an asymmetry in the wiring efficiency associated with the different assemblies. The results indicate the existence of a shorter gap between the FAD cofactor and the PtNCs in the enzymatically implanted assembly, resulting in elevated bioelectrocatalytic currents, lower overpotential, and a higher turnover rate, 2580 e^- s^-1. The implanted assembly is then coupled to a bilirubin oxidase-adsorbed MPCNP cathode to yield an all-DET biofuel cell. Due to the superior electrical contact of the inside-out-synthesized anode, this cell demonstrates enhanced discharge potential and power outputs as compared to similar systems employing electrochemically synthesized outside-in-grown PtNC-GOx/MPCNPs or even GOx-modified MPCNPs diffusionally mediated by ferrocenemethanol.

SUBMITTER: Trifonov A

PROVIDER: S-EPMC9473223 | biostudies-literature | 2019 Jan

REPOSITORIES: biostudies-literature

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Enzymatic self-wiring in nanopores and its application in direct electron transfer biofuel cells.

Trifonov Alexander A Stemmer Andreas A Tel-Vered Ran R

Nanoscale advances 20180906 1

A synthetic enzymatic activity in nanopores leading to the direct fabrication of modified electrodes applicable as biosensors and/or biofuel cell elements is reported. We demonstrate the heterogeneous enzymatic implanting of platinum nanoclusters, PtNCs, in glucose oxidase, GOx, immobilized on mesoporous carbon nanoparticles, MPCNP-modified surface. As the pores confine the growth of the clusters, the PtNC@GOx/MPCNP assembly becomes electrically wired to the matrix, demonstrating direct electron ...[more]

PMID: 36132446

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Project description:The concept that anaerobic microorganisms can directly accept electrons from Fe(0) has been controversial because direct metal-microbe electron transfer has previously only been indirectly inferred. Fe(0) oxidation was studied with Geobacter sulfurreducens strain ACL, an autotrophic strain that was previously shown to grow with electrons derived from a graphite cathode as the sole electron donor. Strain ACL grew with Fe(0) as the sole electron donor and fumarate as the electron acceptor. However, it appeared that at least a portion of the electron transfer was via H2 produced nonenzymatically from the oxidation of Fe(0) to Fe(II). H2, which accumulated in abiotic controls, was consumed during the growth of strain ACL, the cells were predominately planktonic, and genes for the uptake hydrogenase were highly expressed. Strain ACLHF was constructed to prevent growth on H2 or formate by deleting the genes for the uptake of hydrogenase and formate dehydrogenases from strain ACL. Strain ACLHF also grew with Fe(0) as the sole electron donor, but H2 accumulated in the culture, and cells heavily colonized Fe(0) surfaces with no visible planktonic growth. Transcriptomics suggested that the outer surface c-type cytochromes OmcS and OmcZ were important during growth of strain ACLHF on Fe(0). Strain ACLHF did not grow on Fe(0) if the gene for either of these cytochromes was deleted. The specific attachment of strain ACLHF to Fe(0), coupled with requirements for known extracellular electrical contacts, suggest that direct metal-microbe electron transfer is the most likely option for Fe(0) serving as an electron donor.IMPORTANCE The anaerobic corrosion of iron structures is expensive to repair and can be a safety and environmental concern. It has been known for over 100 years that the presence of anaerobic respiratory microorganisms can accelerate iron corrosion. Multiple studies have suggested that there are sulfate reducers, methanogens, and acetogens that can directly accept electrons from Fe(0) to support sulfate or carbon dioxide reduction. However, all of the strains studied can also use H2 as an electron donor for growth, which is known to be abiotically produced from Fe(0). Furthermore, no proteins definitely shown to function as extracellular electrical contacts with Fe(0) were identified. The studies described here demonstrate that direct electron transfer from Fe(0) can support anaerobic respiration. They also map out a simple genetic approach to the study of iron corrosion mechanisms in other microorganisms. A better understanding of how microorganisms promote iron corrosion is expected to lead to the development of strategies that can help reduce adverse impacts from this process.

Dataset Information

Enzymatic self-wiring in nanopores and its application in direct electron transfer biofuel cells.

Publications

Enzymatic self-wiring in nanopores and its application in direct electron transfer biofuel cells.

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