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Iron-based nanomaterials (NMs) are increasingly used to promote extracellular electron transfer (EET) for energy production in bioelectrochemical systems (BESs). However, the composition and roles of planktonic bacteria in the solution regulated by iron-based NMs have rarely been taken into account. Herein, the changes of the microbial community in the solution by S-doped NiFe2O4 anodes have been demonstrated and used for constructing electroactive consortia on normal carbon cloth anodes, which could achieve the same level of electricity generation as NMs-mediated biofilm, as indicated by the significantly high voltage response (0.64 V) and power density (3.5 W m−2), whereas with different microbial diversity and connections. Network analysis showed that the introduction of iron-based NMs made Geobacter positively interact with f_Rhodocyclaceae, improving the competitiveness of the consortium (Geobacter and f_Rhodocyclaceae). Additionally, planktonic bacteria regulated by S-doped anode alone cannot hinder the stimulation of Geobacter by electricity and acetate, while the assistance of lining biofilm enhanced the cooperation of sulfur-oxidizing bacteria (SOB) and fermentative bacteria (FB), thus promoting the electroactivity of microbial consortia. This study reveals the effect of S-doped NiFe2O4 NMs on the network of microbial communities in MFCs and highlights the importance of globality of microbial community, which provides a feasible solution for the safer and more economical environmental applications of NMs.

S-Doped NiFe2O4 Nanosheets Regulated Microbial Community of Suspension for Constructing High Electroactive Consortia