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Surface modification of electrodes with glycans was investigated as a strategy for modulating the development of electrocatalytic biofilms for microbial fuel cell applications. Covalent attachment of phenyl-mannoside and phenyl-lactoside adlayers on graphite rod electrodes was achieved via electrochemically assisted grafting of aryldiazonium cations from solution. To test the effects of the specific bio-functionalities, modified and unmodified graphite rods were used as anodes in two-chamber microbial fuel cell devices. Devices were set up with wastewater as inoculum and acetate as nutrient and their performance, in terms of output potential (open circuit and 1 kΩ load) and peak power output, was monitored over two months. The presence of glycans was found to lead to significant differences in startup times and peak power outputs. Lactosides were found to inhibit the development of biofilms when compared to bare graphite. Mannosides were found, instead, to promote exoelectrogenic biofilm adhesion and anode colonization, a finding that is supported by quartz crystal microbalance experiments in inoculum media. These differences were observed despite both adlayers possessing thickness in the nm range and similar hydrophilic character. This suggests that specific glycan-mediated bioaffinity interactions can be leveraged to direct the development of biotic electrocatalysts in bioelectrochemical systems and microbial fuel cell devices.

Cost‐effective electrode materials to be used as cathodes in lab‐scale prototype microbial fuel cells (MFCs) were prepared from mixtures of carbon black (C) and zirconium oxide (ZrO2) of different composition. The catalytic activity of these cathodes in the oxygen reduction reaction (ORR) and their stability toward poisoning in typical MFC operative conditions were assessed by using electrochemical techniques. Scanning electron microscopy and Brunauer–Emmett–Teller measurements gave insights into sample morphology and surface area. The results indicated that the C/ZrO2 sample with a ZrO2 loading of 25 wt % (C/ZrO2_25) represents the best compromise in terms of ORR activity and stability. C/ZrO2_25 was assembled into cathodes of a prototype single‐chamber MFC, which produced a maximum power density of 600 mW m−2. A comparative cost analysis of energy production indicated that the cost of energy delivered by MFCs assembled with a C/ZrO2 cathode was more than 15 times lower than that of MFCs assembled with a reference Pt/C cathode. Less film, more power: Mixtures of carbon black (C) and zirconium oxide (ZrO2) were prepared by ball milling at different ZrO2 loadings (C/ZrO2) for application as cathodes of microbial fuel cells (see figure). The use of ZrO2 was found to have a favorable effect on electrode stability, by inhibiting the adsorption of the main components of feedstock solution and the formation of biofilm at the catalyst layer.