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Efficient Hydrogen Delivery for Microbial Electrosynthesis via 3D-Printed Cathodes.

ABSTRACT: The efficient delivery of electrochemically in situ produced H₂ can be a key advantage of microbial electrosynthesis over traditional gas fermentation. However, the technical details of how to supply large amounts of electric current per volume in a biocompatible manner remain unresolved. Here, we explored for the first time the flexibility of complex 3D-printed custom electrodes to fine tune H₂ delivery during microbial electrosynthesis. Using a model system for H₂-mediated electromethanogenesis comprised of 3D fabricated carbon aerogel cathodes plated with nickel-molybdenum and Methanococcus maripaludis, we showed that novel 3D-printed cathodes facilitated sustained and efficient electromethanogenesis from electricity and CO₂ at an unprecedented volumetric production rate of 2.2 L _CH4 /L _catholyte /day and at a coulombic efficiency of 99%. Importantly, our experiments revealed that the efficiency of this process strongly depends on the current density. At identical total current supplied, larger surface area cathodes enabled higher methane production and minimized escape of H₂. Specifically, low current density (<1 mA/cm²) enabled by high surface area cathodes was found to be critical for fast start-up times of the microbial culture, stable steady state performance, and high coulombic efficiencies. Our data demonstrate that 3D-printing of electrodes presents a promising design tool to mitigate effects of bubble formation and local pH gradients within the boundary layer and, thus, resolve key critical limitations for in situ electron delivery in microbial electrosynthesis.

SUBMITTER: Kracke F

PROVIDER: S-EPMC8369483 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:Hydrogen-entangled electron transfer has been verified as an important extracellular pathway of sharing reducing equivalents to regulate biofilm activities within a diversely anaerobic environment, especially in microbial electrosynthesis systems. However, with a lack of useful methods for in situ hydrogen detection in cathodic biofilms, the role of hydrogen involvement in electron transfer is still debatable. Here, a cathodic biofilm was constructed in CH4-produced microbial electrosynthesis reactors, in which the hydrogen evolution dynamic was analyzed to confirm the presence of hydrogen-associated electron transfer near the cathode within a micrometer scale. Fluorescent in situ hybridization images indicated that a colocalized community of archaea and bacteria developed within a 58.10-?m-thick biofilm at the cathode, suggesting that the hydrogen gradient detected by the microsensor was consumed by the collaboration of bacteria and archaea. Coupling of a microsensor and cyclic voltammetry test further provided semiquantitative results of the hydrogen-associated contribution to methane generation (around 21.20% ± 1.57% at a potential of -0.5 V to -0.69 V). This finding provides deep insight into the mechanism of electron transfer in biofilm on conductive materials.IMPORTANCE Electron transfer from an electrode to biofilm is of great interest to the fields of microbial electrochemical technology, bioremediation, and methanogenesis. It has a promising potential application to boost more value-added products or pollutant degradation. Importantly, the ability of microbes to obtain electrons from electrodes and utilize them brings new insight into direct interspecies electron transfer during methanogenesis. Previous studies verified the direct pathway of electron transfer from the electrode to a pure-culture bacterium, but it was rarely reported how the methanogenic biofilm of mixed cultures shares electrons by a hydrogen-associated or hydrogen-free pathway. In the current study, a combination method of microsensor and cyclic voltammetry successfully semiquantified the role of hydrogen in electron transfer from an electrode to methanogenic biofilm.

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Efficient Hydrogen Delivery for Microbial Electrosynthesis via 3D-Printed Cathodes.

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