Free nitrous acid-assisted asymmetrical alternating current electrochemistry (FNA-AACE) for multi-heavy metals decontamination in waste activated sludge

Heavy metal contamination of waste activated sludge (WAS) is a key factor limiting the land application of sludge for nutrients recovery. This study proposes a novel free nitrous acid (FNA)-assisted asymmetrical alternating current electrochemistry (FNA-AACE) process to achieve high-efficiency decontamination of multi-heavy metals (Cd, Pb, and Fe) in WAS. The optimal operating conditions, the heavy metal removal performance of FNA-AACE, and the related mechanisms for maintaining the high performance were systematically investigated. During the FNA-AACE process, FNA treatment was optimal with an exposure time of 13 h at a pH of 2.9 and an FNA concentration of 0.6 mg/g TSS. Then the sludge was washed with EDTA in a recirculating leaching system under asymmetrical alternating current electrochemistry (AACE). The 6-h working and the following electrode cleaning were defined as a working circle of AACE. After three cycles of working-cleaning periods in AACE treatment, the cumulative removal efficiency of the toxic metals Cd and Pb reached over 97% and 93%, respectively, whilst that of Fe was greater than 65%. This surpasses most previously reported efficiencies and possesses a shorter treatment duration and sustainable EDTA circulation. The mechanism analysis suggested that FNA pretreatment provoked the migration of heavy metals for leaching enhancement, as well as reduced the demand for EDTA eluent concentration and increased conductivity, which can improve the AACE efficiency. Meanwhile, the AACE process absorbed the anionic chelates of heavy metals and reduced them to zero-valent particles on the electrode, regenerating the EDTA eluent and maintaining its high extraction efficiency for heavy metals. In addition, FNA-AACE could provide different electric field operation modes, allowing it to have flexibility for the real application processes. This proposed process is expected to be coupled with anaerobic digestion in wastewater treatment plants (WWTPs) for high efficiency of heavy metal decontamination, sludge reduction, and resource/energy recovery.