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[Display omitted] • The Zn substituted Co 3 O 4 catalysts were prepared and applied in PMS activation for florfenicol removal. • The Zn substitution induced electron rearrangement and promoted oxygen vacancies formation in Co 3 O 4. • The Zn substituted Co 3 O 4 (Zn 0.03 Co) exhibited superior florfenicol removal and higher reaction rate than Co 3 O 4. • The florfenicol degradation is highly dependent on PMS/Zn 0.03 Co/florfenicol dosage, temperature and initial pH. • The degradation mechanism and routes were proposed combining LC-MS/MS and theoretical calculation results. Florfenicol (FLO) is a broad-spectrum halogenated antibiotic (containing F and Cl atoms), and the discharged FLO in wastewater exhibits potential biotoxicity. Peroxymonosulfate (PMS) activation can generate reactive oxygen species (ROSs) to realize efficient degradation of organic pollutants. Herein, Zn-substituted Co 3 O 4 (Zn x Co) catalysts were prepared and applied in PMS activation for FLO degradation. The physicochemical properties were systematically studied by combining experiments and density functional theory (DFT) calculation. The Zn partial substitution induced electron rearrangement and promoted oxygen vacancy (OV) formation in Co 3 O 4. Zn 0.03 Co catalyst exhibited superior FLO removal, achieving a higher reaction rate of 0.112 min−1 than Co 3 O 4 (0.053 min−1). The FLO degradation was highly dependent on the factors of PMS/Zn 0.03 Co/FLO dosage, temperature, initial pH, and coexisting inorganic anions. The Zn 0.03 Co also displayed outstanding performance in PMS activation for degradation of various typical organic pollutants. Electron paramagnetic resonance (EPR) spectra and quenching experiments indicated that both radical species ( · OH , SO 4 · - , and · O 2 -) and nonradical species (1O 2) contribute to FLO removal. The redox cycle of Co3+/Co2+ and OVs played an essential role in PMS activation. The electron structure of FLO and parameters of PMS adsorbed on Zn x Co were calculated. The longer length of Co O and O O bonds for the adsorbed PMS could enhance its activation to generate ROSs. The intermediates were detected, and five degradation pathways were proposed. The acute and chronic toxicities of intermediates suggested that the dechlorination process is important for the toxicity attenuation of FLO. This study clarified the performance enhancement mechanism of Zn substitution on FLO degradation by PMS activation using Co 3 O 4 based catalyst, which favors the development of PMS-based advanced oxidation processes for wastewater treatment. [ABSTRACT FROM AUTHOR]

The formation of aerobic granular sludge (AGS) is relatively difficult during the treatment of refractory wastewater, which generally shows small granular sizes and poor stability. The formation of AGS is regulated by N-Acyl homoserine lactones (AHLs)-mediated quorum sensing (QS). However, the potential role of AHLs in AGS formation under the toxic stress of refractory pollutants and the heterogeneity in the distribution and function of AHLs across different aggregates are not well understood. This study investigated the potential effects of AHLs on the formation of AGS during phenolic wastewater treatment. The distribution and succession of AHLs across varying granular sizes and development stages of AGS were investigated. Results showed that AGS was successfully formed in 13 days with an average granular size of 335 ± 39 μm and phenol removal efficiency of >99%. The levels of AHLs initially increased and then decreased. C4-HSL and 3-oxo-C10-HSL were enriched in large granules, suggesting they may play a pivotal role in regulating the concentration and composition of extracellular polymeric substances (EPS). The content of EPS constantly increased to 149.4 mg/gVSS, and protein (PN) was enriched in small and large granules. Luteococcus was the dominant genus constituting up to 62% after the granulation process, and exhibited a strong association with C4-HSL. AHLs might also regulate the bacterial community responsible for EPS production, and pollutant removal, and facilitate the proliferation of slow-growing microorganisms, thereby enhancing the formation of AGS. The synthesis and dynamics of AHLs were mainly governed by AHLs-producing bacterial strains of Rhodobacter and Pseudomonas , and AHLs-quenching strains of Flavobacterium and Comamonas. C4-HSL and 3-oxo-C10-HSL might be the major contributors to promoting sludge granulation under phenol stress and play critical roles in large granules. These findings enhance our understanding of the roles that AHLs play in sludge granulation under toxic conditions. [Display omitted] • C4-HSL and 3-oxo-C10-HSL were mainly involved in granular formation. • Concentration of N-Acyl homoserine lactones (AHLs) in large granules was higher. • Protein was more effective in granules formation as compared to polysaccharides. • AHLs regulating functional microflora contributed to granules formation. • Mechanism of AHLs on granular formation under phenol condition was proposed. [ABSTRACT FROM AUTHOR]

• Stable NOB suppression is maintained in MABR treating low-strength wastewater for > 200 days. • Acidic pH of 5.0–5.2 and in situ FNA of 1 mg N/L jointly result in NOB suppression. • An unprecedentedly high AOB activity at around 2.4 kg N/(m3 d) is achieved at a short HRT of a mere 30 min. • Acid-tolerant AOB in MABR-biofilms show different apparent kinetics and responses to environmental factors. Shortcut nitrogen removal holds significant economic appeal for mainstream wastewater treatment. Nevertheless, it is too difficult to achieve the stable suppression of nitrite-oxidizing bacteria (NOB), and simultaneously maintain the activity of ammonia-oxidizing bacteria (AOB). This study proposes to overcome this challenge by employing the novel acid-tolerant AOB, namely " Candidatus Nitrosoglobus", in a membrane-aerated biofilm reactor (MABR). Superior partial nitritation was demonstrated in low-strength wastewater from two aspects. First, the long-term operation (256 days) under the acidic pH range of 5.0 to 5.2 showed the successful NOB washout by the in situ free nitrous acid (FNA) of approximately 1 mg N/L. This was evidenced by the stable nitrite accumulation ratio (NAR) close to 100 % and the disappearance of NOB shown by 16S rRNA gene amplicon sequencing and fluorescence in situ hybridization. Second, oxygen was sufficiently supplied in the MABR, leading to an unprecedentedly high ammonia oxidation rate (AOR) at 2.4 ± 0.1 kg N/(m3 d) at a short hydraulic retention time (HRT) of a mere 30 min. Due to the counter diffusion of substrates, the present acidic MABR displayed a significantly higher apparent oxygen affinity (0.36 ± 0.03 mg O 2 /L), a marginally lower apparent ammonia affinity (14.9 ± 1.9 mg N/L), and a heightened sensitivity to FNA and pH variations, compared with counterparts determined by flocculant acid-tolerant AOB. Beyond supporting the potential application of shortcut nitrogen removal in mainstream wastewater, this study also offers the attractive prospect of intensifying wastewater treatment by markedly reducing the HRT of the aerobic unit. [Display omitted] [ABSTRACT FROM AUTHOR]