Coupled sulfur and electrode-driven autotrophic denitrification for significantly enhanced nitrate removal

Elemental sulfur (S⁰)-based autotrophic denitrification (SAD) has gained intensive attention in the treatment of secondary effluent for its low cost, high efficiency, and good stability. However, in practice, the supplementary addition of limestone is necessary to balance the alkalinity consumption during SAD operation, which increases water hardness and reduces the effective reaction volume. In this study, a coupled sulfur and electrode-driven autotrophic denitrification (SEAD) process was proposed with superior nitrate removal performance, less accumulation of sulfate, and self-balance of acidity-alkalinity capacity by regulating the applied voltage. The dual-channel electron supply from S⁰ and electrodes made the nitrate removal rate constant k in the SEAD process 3.7-5.1 and 1.4-3.5 times higher than that of the single electrode- and sulfur-driven systems, respectively. The S° contributed to 75.3%-83.1% of nitrate removal and the sulfate yield during SEAD (5.67-6.26 mg SO₄²⁻/mg NO₃⁻-N) was decreased by 17%-25% compared with SAD. The S⁰ particle and electrode both as active bio-carriers constructed collaborative denitrification communities and functional genes. Pseudomonas, Ralstonia and Brevundimonas were the dominant denitrifying genera in S⁰ particle biofilm, while Pseudomonas, Chryseobacterium, Pantoea and Comamonas became dominant denitrifying genera in the cathode biofilm. The narG/Z/H/Y/I/V, nxrA/B, napA/B, nirS/K, norB/C and nosZ were potential functional genes for efficient nitrate reduction during the SEAD process. Metagenomic sequencing indicated that S⁰ as an electron donor has greater potential for complete denitrification than the electrode. These findings revealed the potential of SEAD for acting as a highly efficient post denitrification process.