Engineering <i>Shewanella oneidensis</i>‐Carbon Felt Biohybrid Electrode Decorated with Bacterial Cellulose Aerogel‐Electropolymerized Anthraquinone to Boost Energy and Chemicals Production

Interfacial electron transfer between electroactive microorganisms (EAMs) and electrodes underlies a wide range of bio-electrochemical systems with diverse applications. However, the electron transfer rate at the biotic-electrode interface remains low due to high transmembrane and cell-electrode interfacial electron transfer resistance. Herein, a modular engineering strategy is adopted to construct a Shewanella oneidensis-carbon felt biohybrid electrode decorated with bacterial cellulose aerogel-electropolymerized anthraquinone to boost cell-electrode interfacial electron transfer. First, a heterologous riboflavin synthesis and secretion pathway is constructed to increase flavin-mediated transmembrane electron transfer. Second, outer membrane c-Cyts OmcF is screened and optimized via protein engineering strategy to accelerate contacted-based transmembrane electron transfer. Third, a S. oneidensis-carbon felt biohybrid electrode decorated with bacterial cellulose aerogel and electropolymerized anthraquinone is constructed to boost the interfacial electron transfer. As a result, the internal resistance decreased to 42 Ω, 480.8-fold lower than that of the wild-type (WT) S. oneidensis MR-1. The maximum power density reached 4286.6 ± 202.1 mW m^-2, 72.8-fold higher than that of WT. Lastly, the engineered biohybrid electrode exhibited superior abilities for bioelectricity harvest, Cr⁶⁺ reduction, and CO₂ reduction. This study showed that enhancing transmembrane and cell-electrode interfacial electron transfer is a promising way to increase the extracellular electron transfer of EAMs.