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Given the aggravated greenhouse effect caused by CO2 and the current energy shortage, CO2 capture and reuse has been gaining ever-increasing concerns. Microbial Electrolysis Cells (MECs) has been considered to be a promising alternative to recycle CO2 bioelectrochemically to low-carbon electrofuels such as CH4 by combining electroactive microorganisms with electrochemical stimulation, enabling both CO2 fixation and energy recovery. In spite of the numerous efforts dedicated in this field in recent years, there are still many problems that hinder CO2 bioelectroconversion technique from the scaling-up and potential industrialization. This review comprehensively summarized the working principles, extracellular electron transfers behaviors, and the critical factors limiting the wide-spread utilization of CO2 electromethanogenesis. Various characterization and electrochemical testing methods for helping to uncover the underlying mechanisms in CO2 electromethanogenesis have been introduced. In addition, future research needs for pushing forward the development of MECs technology in real-world CO2 fixation and recycling were elaborated.

CO2 bioelectromethanosynthesis represents a promising strategy for the capture and utilization of CO2. In such process, the continuous generation of electron (e-) and proton (H+) in anodic oxidation are of prime importance for the efficient cathodic CO2 electroreduction and process stability. Proton transfer, however, is very easy to be hindered due to the fouling of proton exchange membrane (PEM). In this study, an artificial channel in microbial electrolysis cell (MEC) was proposed to strengthen the transport of protons from anodic to cathodic compartment, and H+-rich anolyte was semi-continuously circulated to the cathodic chamber to provide protons for CO2 electroreduction. The results indicated that the daily CH4 yield in cathode with anolyte circulation (18.5 mL/d·L-reactor) was 5.4-fold higher than that without circulation (2.9 mL/d·L-reactor). Meanwhile, efficient anodic biodegradation of organic components was observed with COD, proteins and polysaccharides removal of up to 95.6 ± 1.9%, 96.3 ± 3.7% and 99.1 ± 0.2% respectively, which supplied a continuous e-/H+ donor for CO2 electroconversion. 16S rRNA gene pyrosequencing analysis identified a large number of proteins-utilizing Bacteroidetes (14.11%) and polysaccharides-consuming Thermotogae (18.49%) in anodic biofilm, conductive to the biodegradation of organic components. Moreover, a high abundance of Methanobacterium (81.07%) was detected to prevail in cathodic biofilm, demonstrating the occurrence of highly enhanced CH4 bioelectrosysthesis. The syntrophic and symbiotic relationship was established in the dual-bioelectrode system, creating a beneficial environment and an energy-efficient approach for biowaste refinery and CO2 electromethanosynthesis.