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Theoretical calculation results showed that the 100 facets exhibited a lower activation energy barrier for oxygen reduction reaction than 001 facets, supporting the experimental observation that 100 facet-dominated HNR had a higher ROS production efficiency than 001 facet-dominated HNP. These results indicated that surface characteristics not only mediated the microbial reduction of Fe(III) but also affected the aerobic oxidation of microbially reduced Fe(II). Accessibility of electron donors to surface iron atom determined the reduction of Fe(III), and act