Search

Owing to the development of urbanization, the amount of sewage sludge generated through biological activated sludge process has increased dramatically. Anaerobic fermentation of sludge is recognized as an expedient and efficient treatment process, widely applied for biogas generation, resource recovery, and volatile fatty acid production. Volatile fatty acids are one of the most widely used carbon sources and have great use in biological nutrient removals. Volatile fatty acids production in anaerobic sludge fermentation is affected by sludge properties, metabolic pathways, and operating parameters. This paper aims to present an overview of the recent advancement in volatile fatty acids production from waste activated sludge. Standalone and hybrid pretreatment methods prior to the sludge fermentation were introduced and assessed based on VFAs accumulation rate and system performance. In addition, different metabolic steps involved in anaerobic fermentation (i.e. hydrolysis, acidification, and methanogenesis) were deeply evaluated. More importantly, the effects of humic substances were evaluated, among which, the electron transfer, the enzyme activity of microbial species, and the interaction between exogenous electron transporters and humic substances were illustrated. Furthermore, the influence of nitrogen and phosphorus ingredients in sludge fermentation and volatile fatty acids production was introduced. It was found that the additives and pretreatment of waste activated sludge are energetically preferred for the hydrolysis improvement and accelerating the volatile fatty acids accumulation. It was concluded that different structures of humic substances may have different effect on the fermentation process and volatile fatty acids production. The synergistic addition of hydrolytic enzymes assisted to reverse the negative effect of humic acids in some cases, and mitigated the adverse effect of humic substances on the inhibition of bacterial growth. The composition and properties of waste activated sludge may limit its biodegradability and hamper the volatile fatty acids production.

Hemin has attracted considerable interest as an efficient catalyst recently, however, its direct application is inefficient due to severe molecular aggregation. Immobilizing hemin on various supports is a feasible approach to address this issue. In this work, a CNTs-hemin catalyst was prepared by loading hemin onto multiwalled carbon nanotubes (CNTs) through ball milling. Compared with hemin, CNTs-hemin demonstrates remarkably enhanced performance in the peroxymonosulfate system, with a 650-fold improvement of apparent rate constant, reaching 97.8% degradation of sulfathiazole in 5 min. High-valent iron-oxo porphyrin cation ((Porp)

Arsenic-alkali residue (AAR) from antimony production can pose significant health and environmental hazards due to the risk of arsenic (As) leaching. In this study, geopolymer composite synthesized from fly ash (FA) was investigated for efficient stabilization of high-arsenic-containing AAR (As

This study investigated the effects of electrical signaling disruption induced by adding tetraethylammonium (TEA, a potassium channel blocker) on the formation of mixed-cultured electroactive biofilms, especially the relative abundance of Geobacter over time. Results showed that TEA addition decelerated the biofilm formation, but selectively enriched Geobacter over time (45.8% on Day 32, 67.7% on Day 60 and 78.1% on Day 90), thus resulting in higher final extracellular electron transfer (EET) efficiency. Redundancy analysis (RDA) confirmed that TEA and operation time were significant factors for the selective enrichment of Geobacter. Moreover, increase in cellular processes and signal processing by PICRUSt analysis indicated adaptive responses of electrogenic biofilms to electrical signaling disruption. Furthermore, qRT-PCR indicated the compensatory roles of key cytochromes and pilA in electrochemical communication, which induced Geobacter enrichment. This work provided a broader understanding of electroactive biofilm regulation and potential applications for electricity generation and biosensor in the future.

A microbial fuel cell-photocatalysis system with a novel photocatalytic air-cathode (MFC-PhotoCat) was proposed for synergistic degradation of 2,4,6-trichlorophenol (TCP) with simultaneous electricity generation. Stable electricity generation of 350 mV was achieved during 130 days of operation. Besides, 50 mg L−1 TCP was completely degraded within 72 h, and the rate constant of 0.050 h−1 was 1.8-fold higher than MFC with air-cathode without N-TiO2 photocatalyst. Degradation pathway was proposed based on the intermediates detected and density functional theory (DFT) calculation, with two open-chain intermediates (2-chloro-4-keto-2-hexenedioic acid and hexanoic acid) detected. Furthermore, hierarchical cluster and PCoA revealed significant shifts of microbial community structures, with enriched exoelectrogen (55.2% of Geobacter) and TCP-degrading microbe (7.1% of Thauera) on the cathode biofilm as well as 61.8% of Pseudomonas in the culture solution. This study provides a promising strategy for synergic degradation of recalcitrant contaminants by intimate-coupling of MFC and photocatalysis.

Biological wastewater treatment generates a large quantity of sewage sludge that requires proper treatments. In this study, the biochar pyrolyzed by sludge conditioned with Fenton's reagent and lime (referred to as Fenton-lime system) was first used as an efficient silicon fertilizer for rice cultivation. When the pyrolysis temperature was 750 °C, the dissolved silicon and available silicon contents in biochar derived from sludge conditioned with Fenton-lime system were much higher than those in raw sludge derived biochar without conditioning (3.49 vs. 0.72, 77.25 vs. 2.33 mg/g dry solid, respectively). The enhanced available silicon content was attributed to the newly formed calcium aluminosilicate from the reactions between the added lime and silicon-rich phases in sludge. The rice cultivated with biochar derived from Fenton-lime conditioned sludge showed improved biomass of stem and root by 76.85% and 36.11%, respectively, compared to blank group without the addition of Si source. Heavy metals and the reactive oxygen species (ROS) accumulation in rice were not observed after a culture period of 30 days in the application of sludge-derived biochar as silicon fertilizer. This study provides a promising approach for sewage sludge recycling as an efficient silicon fertilizer in silicon-deficiency land.

Wet chemical approach is widely applied for P extraction from incinerated sewage sludge ash (ISSA) due to the relatively simple process and low lost. In this study, H2SO4 and H2C2O4 were compared to recover P from ISSA through three steps of acid leaching, cation exchange resin (CER) purification and precipitation. Transformations of P speciation and mineral phases in ISSA from 600 to 900 °C were studied. The results showed that the ISSA samples were mainly composed of inorganic P (IP), and part of non-apatite IP (NAIP, mainly AlPO4) would transform to apatite P (AP, Ca3(PO4)2) with the increase in temperature. The ratio of NAIP to IP dropped from 71.9% at 600 °C to 53.7% at 900 °C. Effect of acid concentration on the leaching efficiency of P from the ISSA samples incinerated at different temperatures by H2SO4 and H2C2O4 was investigated, and the leaching behaviors of key elements of P, Ca, Al and Fe were compared. H2C2O4 exhibited a better performance than H2SO4 for the leaching efficiency of P. Severe sintering of ash particles occurred at temperature >800 °C inhibited the P leaching by H2SO4. During CER purification, the impurity elements in the H2SO4 leachate were easily removed by CER, whereas the Al and Fe elements in the H2C2O4 leachate were hardly removed due to the formation of anionic complexes between Al3+/Fe3+ and oxalic ions. Finally, high-purity struvite product was synthesized from the purified H2SO4 leachate, which could be directly utilized as a fertilizer with negligible environmental risk. Amorphous aluminum and iron hydroxyphosphates were obtained from the H2C2O4 leachate. This study provides insights for P recovery from ISSA samples by different acid leaching systems.

Massive realgar tailings abandoned in mining areas in China have caused serious arsenic (As) pollution seeking for urgent disposal. Stabilization treatment is a feasible strategy, however, stabilization technologies for realgar tailings, that are Fe-deficient, Ca-rich and S-rich, have not been well developed to date. In this study, we conducted a pilot-scale stabilization treatment of realgar tailings via ferrous sulfate addition to evaluate the transformation of As during stabilization. We found that Si, As, Ca, and S were the predominant elements in the raw realgar tailings with a low content of Fe, and realgar (AsII4S4) and pharmacolite (CaHAsVO4·2H2O) were the main As-bearing minerals. After the ferrous sulfate treatment, the As leaching concentration of realgar tailings was successfully reduced from 135 mg/L to a level below the Chinese regulatory limit (2.5 mg/L). Based on the results of leaching tests, sequential extraction analysis, XRD, SEM-EDS, XPS, and thermodynamic modeling, we concluded that ferrous sulfate addition enhanced the transformation of Ca–As and S–As species to more stable Fe–As species, e.g., crystalline symplesite and amorphous Fe–As complex. Dissolution of pharmacolite was facilitated by H+ and SO42− derived from the hydrolysis and oxidation of ferrous sulfate, and oxidation of realgar could be promoted by reactive oxygen species (ROSs) from Fe(II) oxygenation. This study improved our understanding of As transformation pathways in realgar tailings during ferrous sulfate treatment, which could serve as an alternative scheme for realgar tailings stabilization.

In this study, a method to reduce the emission of NOx precursors (e.g., hydrogen cyanide (HCN) and ammonia (NH3)) while simultaneously reclaim more plant-available P was proposed through pyrolyzing ferric sludge (sludge conditioned by Fenton's reagents) rather than raw sludge. The nitrogen and phosphorus transformation at different pyrolysis temperatures was investigated. The results indicated that in comparison with the pyrolysis of raw sludge, the remaining iron compounds in ferric sludge can fix char-N in more stable forms (e.g., appearance of pyrrole-N at 900 °C). The secondary cracking of amine-N compounds in tar-N (e.g., 81.67% increase of amine-N at 900 °C) can be inhibited. Hence, more amine-N was remained and less heterocyclic-N and nitrile-N compounds were generated in tar N. Less generation of NH3-N and HCN-N was also observed in NOx precursors (e.g., 5.46% decrease of NH3-N and 6.91% decrease of HCN-N at 900 °C). Moreover, the results of X-ray diffractometry, liquid 31P nuclear magnetic resonance spectroscopic, X-ray photoelectron spectroscopic, and chemical analyses collectively indicated that iron present in ferric sludge also favored reclamation of more plant-available P. In comparison with the pyrolysis of raw sludge, an increase in the total phosphorus pool was noted (18.06–36.26 versus 15.54–30.59 mg g−1 dry solids). A decrease in mobility with the predominant P as sodium hydroxide (NaOH)-P, and an increase in plant-available P can be also obtained. This study indicated that pyrolysis of ferric sludge was a feasible way to simultaneously reduce emission of NOx precursors, reclaim plant-available P, and reuse ferric sludge.

Pre-oxidation is effective in enhancing sludge dewaterability. Different types and doses of oxidants are used to improve sludge dewaterability in pre-oxidation. Rapid evaluation of the sludge dewaterability is vital for optimizing the type and dose of oxidants in pre-oxidation. It normally takes more time to evaluate sludge dewaterability by measuring typical indicators such as specific resistance to filtration (SRF), content of bound water, and composition of EPS. This study presented a rapid parameter, oxidation-reduction potential (ORP), to correlate it with the dewaterability of pre-oxidized sludge samples. An index of ΔORP (ΔORP = ORPt=0.5 min–ORPt=0 min) showed positive correlations with SRF (r = 0.89, p

Cell lysis in sludge pretreatment by advanced oxidation process (AOP) has a great effect on sludge dewaterability. Cell lysis caused by reactive radicals (e.g. hydroxyl radical) was dependent on the reaction site of AOP. However, little is known about the accurate radical generation site of AOP in sludge pretreatment. In this study, two kinds of oxidation behaviors from different oxidants (HOCl vs. H2O2) catalyzed by ferrous iron were comparatively investigated. Higher amount of living cells (84.3%) and hydroxyl radicals (9.86 × 10−5 M), and more fragmentized sludge flocs (particle sizes of D50 was 50.1 vs. 57.3 μm of RS) were detected in sludge conditioned by Fe2+/H2O2, which implied that Fenton reaction mainly happened at surface and outside of sludge flocs (such as EPS layer and liquid phase). Thus, it could be regarded as “extracellular oxidation”. Fewer living cells (undetectable), fewer amount of hydroxyl radicals (undetectable in sludge), and more integrated sludge flocs (particle size of D50 was 56.1 vs. 57.3 μm of RS) were determined in sludge conditioned by Fe2+/Ca(ClO)2. Hence, it could be regarded as “Intracellular oxidation”. In addition, sludge pretreatment based on Fe2+/Ca(ClO)2 could achieve simultaneous deep-dewatering performance and total coliforms inactivation. Based on response surface methodology, the optimal dosages of Fe2+ and Ca(ClO)2 were proposed as 106.1 and 234.5 mg/g volatile solids respectively, without any acidification of sludge. Under these optimal dosages, the water content of dewatered sludge cake was 51.9 ± 0.1 wt% and the pH of the final filtrate was 5.8 ± 0.2. Total coliforms of sludge could be inactivated in 10 s after Fe2+/Ca(ClO)2 addition.

Bio-electro-Fenton (BEF) system holds great potential for sustainable degradation of refractory organics. Activated carbon (AC) air cathode was modified by co-pyrolyzing of AC with glucose and doping with nano-zero-valent iron (denoted as nZVI@MAC) in order to promote two-electron oxygen reduction reaction (2e- ORR) for enhanced oxidizing performance. Single chamber microbial fuel cells (SCMFCs) with nZVI@MAC cathode was examined to degrade landfill leachate. It was revealed that nZVI@MAC cathode SCMFC showed higher degradation efficiency towards landfill leachate. Six landfill leachate treatment cycles indicated that nZVI@MAC cathode SCMFC exhibited higher COD removal efficiencies over AC and nZVI@AC and greatly enhanced columbic efficiency compared to AC and nZVI@AC cathode. Anti-biofouling effect was found on nZVI@MAC cathode because of the high Fenton oxidation effects at the vicinity of the cathode. Electrochemical characterizations indicated that MAC cathode had superior 2e- ORR capability than AC and nZVI@AC cathode, which was further evidenced by higher H2O2 production from nZVI@MAC cathode in SCMFC. Graphitic structure of MAC was evidenced by High Resolution Transmission Electron Microscopy, and glucose pyrolysis also resulted in nano carbon spheres on the activated carbon skeletons. Raman spectra indicated more defects were generated on MAC during its co-pyrolyzation with glucose.

Microplastic accumulation in agricultural soils can stress plants and affects quality of the products. Current research on the effects of microplastics on plants is not consistent and the underlying mechanisms are yet unknown. Here, the molecular mechanisms of the stress response were investigated via metabolomic and transcriptomic analyses of rice Oryza sativa L. II Y900 and XS123 under the exposure of polystyrene microplastics (PS-MPs) in a field study. Distinct responses were obtained in these two rice subspecies, showing decreased head rice yield by 10.62% in Y900 and increase by 6.35% in XS123. The metabolomics results showed that PS-MPs exposure inhibited 29.63% of the substance accumulation-related metabolic pathways and 43.25% of the energy expenditure-related metabolic pathways in the Y900 grains; however, these related pathways were promoted in the XS123 grains. The transcriptomics results indicated that the expression of genes encoding proteins involved in the tricarboxylic acid cycle in the Y900 grains was inhibited, but it was enhanced in the XS123 grains. The XS123 subspecies could response against microplastic exposure stress through the metabolite accumulation and energy expenditure pathways, while the Y900 could not. The results provide insight into the perturbation of rice grains in farmlands with microplastics contamination.

Microbial fuel cell (MFC) sensor exhibits attractive prospects for online monitoring of water toxicity as an early warning device. However, the accumulation of dead cells in anode biofilm might decrease the sensing sensitivity of MFC during long term operation. In addition, with repeated exposure to toxins, the microbial community of anode biofilm would also adjust to build up higher endurance to environmental toxicity. In this study, the long term sensing sensitivity of MFC sensor and the microbial community changes were characterized with Pb2+ as the target toxin. The results show that newly formed biofilm with higher live/dead cell ratio exhibited higher sensitivity than mature biofilm. Modification of anodic biofilm via high current stimulation was applied to increase the ratio of live cells, which led to enhanced sensing sensitivity of MFC with mature anode biofilm. However, the enhancement was relatively limited for biofilm that was previously exposed to repeated Pb2+ shocks. Microbial community analysis revealed that the proportions of microbial species possessing higher environmental robustness, such as Hyphomicrobiaceae and Cloacibacillus, significantly increased in the anode biofilm after long term repeated Pb2+ shocks.

Oxidation ditches (ODs) are often used for wastewater treatment. However, limitations of ODs like high energy expenditure and increased sludge sedimentation hinder its wide application. In this study, the computational fluid dynamics (CFD) model integrated with Activated Sludge Model No. 2 (ASM2) was proposed and applied in a full-scale OD. The integrated model provided heterogeneous information on the characteristics of hydrodynamics and biokinetics of OD, especially with respect to the simulation of total phosphorus removal by CFD-ASM2 integration model for the first time. The simulated values of flow velocities, suspended solids (SS), dissolved oxygen, chemical oxygen demand, total nitrogen, ammonium nitrogen, and total phosphorus concentrations were well validated with the measured results, with the standard deviation errors of less than 5.56%, 0.28%, 0.74%, 7.39%, 3.17%, 5.27%, and 7.40%, respectively. Based on the integrated model, four different operational strategies were simulated. The proposed operational strategy of operating 7 surface aerators and 10 submerged impellers not only met the standard discharge requirements (GB 18918-2002) but also consumed less energy by 22.3%, compared with the original strategy of operating 9 surface aerators and 13 submerged impellers. Meanwhile, this proposed operational strategy also reduced the SS concentrations in the second and fourth channels, which was beneficial to elimination of sludge sedimentation. Moreover, the proposed operational strategy was successfully applied and validated in full-scale OD. The foregoing results collectively suggest that the CFD-AMS2 integration model is numerically capable to optimize the operational strategy of ODs.

A hybrid sludge conditioning strategy with electrooxidation and Fe(II) addition was used for heavy metal removal from sewage sludge and industrial sludge, with simultaneous sludge dewatering and stabilization. With the addition of 82 mg/g DS Fe(II) and treatment time of 4.5 h, heavy metal removals of 72.95% and 78.49% for Cu, 66.29% and 84.26% for Zn, and 36.52% and 36.99% for Pb were achieved from sewage sludge and industrial sludge samples respectively. The system pH decreased to 2.33 and 2.98 and the oxidation–reduction potential (ORP) values increased to 435.90 mV and 480.60 mV in sewage sludge and industrial sludge samples, respectively, which was conducive to the desorption and dissolution of heavy metals from sludge structures and the degradation of the organic compounds that complexed with heavy metals. In addition, the hybrid conditioning process demonstrated excellent dewatering performance due to the efficient electrochemical disintegration of sludge flocs together with the coagulation of sludge particles by Fe(III) generated via electrooxidation. The strong acidic and oxidative environment produced by the enhanced electrooxidation process was also responsible for pathogen inactivation.

Over half of century, sanitary landfill was and is still the most economical treatment strategy for solid waste disposal, but the environmental risks associated with the leachate have brought attention of scientists for its proper treatment to avoid surface and ground water deterioration. Most of the treatment technologies are energy-negative and cost intensive processes, which are unable to meet current environmental regulations. There are continuous demands of alternatives concomitant with positive energy and high effluent quality. Microbial fuel cells (MFCs) were launched in the last two decades as a potential treatment technology with bioelectricity generation accompanied with simultaneous carbon and nutrient removal. This study reviews capability and mechanisms of carbon, nitrogen and phosphorous removal from landfill leachate through MFC technology, as well as summarizes and discusses the recent advances of standalone and hybrid MFCs performances in landfill leachate (LFL) treatment. Recent improvements and synergetic effect of hybrid MFC technology upon the increasing of power densities, organic and nutrient removal, and future challenges were discussed in details.

The utilization of recycled biochar combined with chemical leaching is an appropriate method to remove cadmium (Cd) from paddy soil. Some Cd-rich soil clay particulates (particulate Cd) are reported to be removed via biochar adsorption and the potential impact of biochar on soil properties need further study. The removal efficiencies and mechanisms of Cd from soil by using floatable hydroxyapatite modified biochar (HBC) combined with CaCl2 were studied. Synergetic removal efficiencies of total Cd (46.5%) and bioavailable Cd (37.9%) from the paddy soil were achieved with 2% HBC and 1 mM CaCl2. The increased soluble Cd in soil pore water by CaCl2 leaching could be efficiently adsorbed on HBC, and removed by HBC collection, reducing the risk of the residual soluble Cd in soil pore water to rice plants caused by the inefficient drainage in the field. The suspendability of clay particulates in overlying water was little affected by the low-level CaCl2 based on Derjaguin-Landau-Verwey-Overbeek (DLVO) calculation. Moreover, low-level CaCl2 facilitated the accumulation of particulate Cd on the floating HBC via decreasing the interaction energy (by 25%) between clay particulates and HBC. HBC-mediated Cd migration contributed ~70% of total Cd removal, while soluble and particulate Cd removed through the drainage accounted for ~30%. Soil clay proportion maintained at 25.3% due to the replenishment of HBC residues. In addition, soil nutrient and physicochemical conditions were improved with HBC residues. This work provides a novel soil remediation method by using floatable biochar combined with low-level CaCl2 for Cd-contaminated paddy soil remediation.

The evaluation of ecological risks of contaminant mixtures to organisms is very challenging due to the non-linear response of organisms to each component, especially under the co-existence of both stimulators and inhibitors. Whether the stimulatory effect can reduce or even offset the inhibitory effect would be critical to the risk assessment and the treatment measures of mixed pollutants. Here, the combined toxicity of sodium fluoride (NaF), a stimulator with stimulation rate >100%, and six compounds that cannot induce hormesis (four ionic liquids (ILs) and two pesticides) were studied. The time-dependent toxicity of each toxicant on Vibrio qinghaiensis sp.-Q67 was investigated at 0.25, 2, 4, 6, 8, 10 and 12 h. Results showed that four ILs and two pesticides failed to induce hormesis, while NaF induced hormesis from 2 to 6 h and induced stimulation only after 6 h and reached its maximum (650%) at 12 h. All mixture rays with NaF induced hormesis at different times. In the four NaF-IL mixture systems, the absolute value of maximum stimulation demonstrated an upwards and then a downwards trend with the increasing of mixture ratio of IL. In two NaF-pesticide systems, the maximum stimulation effect declined with the increasing of the mixture ratio of pesticide. The toxicities of the mixture were successfully predicted by the improved inverse distance weighted interpolation, which are not able to be predicted by the commonly used concentration addition or independent action models. This paper shed lights on evaluating the hormesis of mixtures and the ecological risk of fluoride.

A hybrid electrochemical conditioning strategy for enhanced sewage sludge dewatering was proposed. A water content of 47.2 wt.% for the dewatered sludge cake was achieved at an applied voltage of 20 V for 30 min, which was significantly lower than previously reported results. The capillary suction time (CST) and specific resistance to filtration (SRF) were decreased by 75.6% and 90.9%, respectively. Four simultaneous processes, including electrooxidation, the electro-Fenton process, molecular oxygen activation via zero valent iron (ZVI) and Fe(III) flocculation, had synergetic effects on the degradation of extracellular polymeric substances (EPS) to enhance sludge dewaterability. The in situ generation of ZVI on the cathode electrode facilitated the reduction of Fe(III) to Fe(II) via activation of molecular oxygen. The sludge pH decreased spontaneously and remained acidic due to the competitive reaction of ZVI generation to hydrogen evolution as well as the Fe(III) flocculation process, which further guaranteed the high efficiency of hydroxyl radical generation. Changes in the physiochemical properties of the sludge (particle size distribution, zeta potential, viscosity and EPS characteristics) induced by the hybrid conditioning process were further explored. In addition, the economic potential of the hybrid system was preliminarily assessed (USD$ 127.6/ton dry sludge).

Microbial fuel cells (MFCs) are promising biotechnologies tool to harvest electricity by decomposing organic matter in waste water, and the anode material is a critical factor in determining the performance of MFCs. In this study, chestnut shell is proposed as a novel anode material with mesoporous and microporous structure prepared via a simple carbonization procedure followed by an activation process. The chemical activation process successfully modified the macroporous structure, created more mesoporous and microporous structure and decreased the O−content and pyridinic/pyrrolic N groups on the biomass anode, which were beneficial for improving charge transfer efficiency between the anode surface and microbial biofilm. The MFC with activated biomass anode achieved a maximum power density (23.6 W m−3) 2.3 times higher than carbon cloth anode (10.4 W m−3). This study introduces a promising and feasible strategy for the fabrication of high performance anodes for MFCs derived from cost-effective, sustainable natural materials.

Sustained molecular oxygen activation by iron doped silicon carbide (Fe/SiC) was investigated under microwave (MW) irradiation. The catalytic performance of Fe/SiC for norfloxacin (NOR) degradation was also studied. Rapid mineralization in neutral solution was observed with a pseudo-first-order rate constant of 0.2239 min −1 under 540 W of MW irradiation for 20 min. Increasing Fe/SiC rod and MW power significantly enhanced the degradation and mineralization rate with higher yield of reactive oxygen species (ROS). Fe shell corrosion and subsequent Fe 0/II oxidation by molecular oxygen with MW activation was the key factor for NOR degradation through two-electron-transfer by Fe 0 under acidic conditions and single-electron-transfer by Fe II under neutral-alkaline solution. Removal rate of NOR was significantly affected by solution pH, showing higher degradation rates at both acidic and alkaline conditions. The highest removal efficiencies and rates at alkaline pH values were ascribed to the contribution of bound Fe II species on the Fe shell surface due to the hydroxylation of Fe/SiC. ·OH was the main oxidizing specie for NOR degradation, confirmed by density functional theory (DFT) calculations and radical scavenger tests. DFT calculations were conducted on the reaction/activation energies of the transition/final states of NOR/degradation products, combined with intermediate identification with high performance liquid chromatography coupled with a triple-quadruple mass spectrometer (HPLC-MS/MS), the piperazinyl ring was the most reactive site for ·OH attack, followed by further ring-opening and stepwise oxidation. In this study, Fe/SiC were proved to be an excellent catalyst for the treatment of fluoroquinolone antibiotics with MW activation.

The electrogeneration of H2O2 and electro-regeneration of ferrous are conflicting matters in electro-Fenton system. In this research, the degradation of Rhodamine B, methyl orange (MO) and 4-chlorophenol (4-CP) was investigated using a novel dual-cathode microbial fuel cell (MFC) electro-Fenton (EF) hybrid system. An air-cathode of an EF system was used for H2O2 electrogeneration and a carbon felt cathode of a MFC was used to accelerate Fe2+ regeneration. Synergistic improvement of MFC power generation and the degradation of the above refractory organics through EF reaction was achieved. The EF air-cathode was fabricated by adopting activated carbon/graphite powder mixture and PVDF binder, which showed higher H2O2 generation but slower Fe3+ reduction rate than MFC carbon felt cathode. The Rhodamine B removal rate constant and mineralization current efficiency of the MFC coupled EF were 64% and 42% higher than that of uncoupled EF, respectively. The MFC-EF coupled system also exhibited significantly higher removal efficiency for MO and 4-CP than that of un-coupled EF system. Moreover, the power density of MFC was greatly enhanced by coupling EF due to higher Fe3+/Fe2+ redox potential than oxygen reduction.

This study investigated the synergistic effect of water content and a composite conditioner of Fenton's reagent combined with red mud (Fenton-RM) on the pyrolytic products (fuel gas, tar, and solid char) of deep-dewatered sludge. The catalytic effect of metal oxides in Fenton-RM could be promoted by the presence of water during sludge pyrolysis, showing higher gas yield with increased water content. Maximum gas outputs of the deep-dewatered sludge conditioned with Fenton-RM (S-Fenton-RM) and the conventional dewatered sludge conditioned with polyacrylamide (S-PAM), both appeared at 900 °C with a water content of 65 wt%, and were 0.257 and 0.189 L/g dry solid (DS), respectively. At the same temperature and with the same water content, the hydrogen (H2) yields of the S-Fenton-RM samples were always higher than those of the S-PAM samples. At 900 °C, the maximum H2 yield of the S-Fenton-RM samples was 0.102 L/g DS, which was 85.5% higher than that of the S-PAM samples. The results indicated that water in the wet sludge provided the steam atmosphere for pyrolysis, and the water vapor then involved in secondary cracking reformation of tar and char gasification reactions, which would be catalyzed by the presence of metal oxides in the Fenton-RM conditioner, thus increasing the yield of fuel gas, especially hydrogen. The H2 production cost from the S-Fenton-RM system is less than that from the S-PAM system. The results suggest that pyrolysis of the wet deep-dewatered sludge conditioned with Fenton-RM is an economical and promising alternative for sewage sludge dewatering and disposal/reuse.

Electro-dewatering (EDW) is an innovative method for volume reduction of sewage sludge before re-utilization and disposal. In this study, dewaterability limit and energy consumption in sludge electro-dewatering process were directly explored using in-situ linear sweep voltammetry (LSV) analysis by a high-voltage electrochemical workstation instead of a traditional DC power source. Dewaterability limits of biosolids EDW were identified under a constant-voltage dewatering mode with different applied voltages at 10, 20, 30, 40, and 50 V, independently. The LSV tests reveal that the dewaterability limit of sludge is attributed to the higher electrical resistance of the sludge layer near the anode. The mass of the filtrate flow was linearly proportional to the total amount of electric charge corresponding to the energy consumption in EDW, which elucidated the principal mechanism of EDW. Under a constant-voltage dewatering mode, the applied voltage is a key factor in controlling the energy consumption. Reducing the applied voltage while extending the dewatering time is proposed to reduce the energy consumption and obtain a good dewatering result. As the applied voltage decreased from 50 to 10 V, the energy consumption could be reduced from 403.6 to 80.3 kWh/m 3 removed water, the dewatering times was increased from 6.4 to 85.4 min, and the dry solids content of dewatered cake increased from 16.1 to 34.4 wt%. Those results indicate that LSV is an effective method to reveal the mechanism of EDW and optimize the operation parameters to reduce energy consumption.

It is urgent to develop recycled ionic liquids (ILs) as green solvents for sustainable biomass pretreatment. The goal of this study is to explore the availability and performance of reusing 1-allyl-3-methylimidazolium chloride ([amim]Cl) and 1-butyl-3-methylimidazolium acetate ([bmim]OAc) for pretreatment, structural evolution, and enzymatic hydrolysis of eucalyptus. Cellulose enzymatic digestibility slightly decreased with the increased number of pretreatment recycles. The hydrolysis efficiencies of eucalyptus pretreated via 4th recycled ILs were 54.3% for [amim]Cl and 72.8% for [bmim]OAc, which were 5.0 and 6.7-folds higher than that of untreated eucalyptus. Deteriorations of ILs were observed by the relatively lower sugar conversion and lignin removal from eucalyptus after 4th reuse. No appreciable changes in fundamental framework and thermal stability of [amim]Cl were observed even after successive pretreatments, whereas the anionic structure of [bmim]OAc was destroyed or replaced. This study suggested that the biomass pretreatment with recycled ILs was a potential alternative for low-cost biorefinery.

In this study, the long-term stability of Cr(VI) in the FeSO4 and H2SO4 (FeSO4-H2SO4) treated chromite ore processing residue (COPR) after 400 curing days and the stabilization mechanisms were investigated. FeSO4-H2SO4 treatment significantly reduced toxicity characteristic leaching procedure (TCLP) and synthetic precipitation leaching procedure (SPLP) Cr(VI) concentrations to lower than the regulatory limit of 1.5mgL-1 (HJ/T 301-2007, China EPA) even for the samples curing 400days, achieving an outstanding long-term stability. Our independent leaching tests revealed that H+ and SO42- have synergistic effect on promoting the release of Cr(VI), which would make Cr(VI) easier accessed by Fe(II) during stabilization. The contributions of H+ and SO42- to Cr(VI) release ratio were 25%-44% and 19%-38%, respectively, as 5mol H2SO4 per kg COPR was used. X-ray powder diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and alkaline digestion analyses were also employed to interpret the possible stabilization mechanism. Cr(VI) released from COPR solid was reduced to Cr(III) by Fe(II), and then formed stable FexCr(1-x)(OH)3 precipitate. This study provides a facile and reliable scheme for COPR stabilization, and verifies the excellent long-term stability of the FeSO4-H2SO4 treated COPR.

During advanced oxidation treatment for enhancing sludge dewaterability, the peptide chains of protein can be decomposed into amino acids. Protein exhibits a great impact on sewage sludge dewaterability. However, the role of amino acids in sludge dewatering remains unclear. In this study, among the 23 types of amino acids investigated, tryptophane (Trp) and lysine (Lys) were identified as the key amino acids affecting sludge dewaterability during Fenton oxidation treatment. The content of lysine showed positive correlations with capillary suction time (CST), specific resistance to filtration (SRF), and bound water content, and the concentrations of total protein, low molecular weight protein, amines and amides, and 3-turn helix of proteinaceous compounds in bound extracellular polymeric substances (EPS), while the content of tryptophane showed negative correlations with the above parameters. The amino acids may be sourced from damage of the membrane and ribosomal proteins by hydroxyl radicals, and the peptide bonds connected with tryptophane were more inclined to be decomposed than other amino acids. Particularly, more amino acids of tryptophane can result in more hydrophobic interaction, and less necessary energy barrier for aggregation of particles. As such, regulating protein degradation towards production of tryptophane may be related with enhanced sludge dewaterability by Fenton oxidation treatment.

Biogas and phosphorus recovery from waste activated sludge (WAS) with sequential homogeneous protocatechuic acid (PCA) enhanced Fenton pretreatment, anaerobic digestion (AD) and microbial electrolysis cell (MEC) were investigated. The cumulation of biogas production of WAS-Fenton-AD was 330.4 mL/g VS, which was 2.05-fold of the control without pretreatment (WAS-AD) during anaerobic digestion. Biogas production of 178 mL/L/d from WAS-Fenton-AD-MEC was achieved, which was 5.23-fold of the WAS-MEC, 2.28-fold of WAS-Fenton-MEC and 1.46-fold of WAS-AD-MEC, respectively. Enhanced phosphorus recovery in form of struvite reached 1.72 g/g TS (18.03% of total P) with a purity of 74.4%. Microbial community richness and diversity analysis revealed that the pretreatment process under circumneutral condition improved the diversity of microbial community, which was consisted of Bacteroidetes (33.90%), Proteobacteria (33.14%), and Chloroflexi (10.14%), compared to a majority of Firmicutes (70.81%) in WAS-AD. This study provides a feasible strategy for the recovery of biogas combined with phosphorus from WAS.

A microbial fuel cell system with intimately coupled photocatalytic-electrogenic anode (photocatalytic-MFC) was proposed for the synergetic degradation of 2,4,6-trichlorophenol (2,4,6-TCP) which has a structure of three chlorine groups connecting to a phenol ring and is well recognized as a recalcitrant pollutant for its high toxicity, bioaccumulation and persistence. The photocatalytic-electrogenic anode was prepared by coating mpg-C3N4 on a carbon felt anode, followed by inoculating with municipal sewage and acclimating with 2,4,6-TCP at gradient concentrations. Improved TCP degradation was achieved, showing 79.3% of TCP removal in 10 h with an original concentration of 200 mg L−1, which was higher than that obtained with the unilluminated MFC (66.0%) and the photocatalytic-only process (56.1%). The coupled photocatalytic-electrogenic process demonstrated different degradation pathways compared with the photocatalytic-only process, with one open-chain compound (2-chloro-4-keto-2-hexenedioic acid, 2-CMA) detected in the photocatalytic-MFC system. Microbial community analysis revealed that Pseudomonas, instead of Geobacter observed in the unilluminated MFC bioanode, dominated in the photocatalytic-electrogenic anode MFC biofilm, which might be responsible for enhanced current generation in the coupled system. In addition, biofilm rich with Rhodococcus on air-cathode was also responsible for the enhanced TCP removal. This research provides an efficient strategy for the treatment of wastewater with recalcitrant contaminants by intimate-coupling of the photocatalytic and the electrogenic processes.

A liquid–gas two-phase computational fluid dynamics (CFD) model was developed to simulate flow field and gas hold-up in a pilot-scale oxidation ditch (OD). The volume of fluid (VOF) model and the mass flow inlet boundary condition for gas injection were introduced in this model. The simulated values of the flow velocities and the gas hold-up were verified by experimental measurements in the pilot-scale OD. The results showed that the gas hold-up at test-site 3, immediately downstream of the surface aerator, was the highest among all three test-sites. Most of the gas existed in the upper portion of the ditch and was close to the inner side of the channel. Based on the liquid–gas two-phase CFD model, three operating conditions with different setting height ratios of the submerged impellers were simulated. The simulated results suggested that the setting heights of the submerged impellers have significant impacts on the flow velocity distribution. Lowering the setting height could increase the flow velocity in the pilot-scale OD. An optimal setting height ratio of 0.273 was proposed, which would be beneficial for minimizing sludge sedimentation, especially near the inner side of the curve bend.

A hybrid electrochemical process with Ca(ClO)2 addition for simultaneous sludge dewaterability, stabilization and phosphorus fixation was proposed. Under optimal conditions (150 mg/g VS Ca(ClO)2, 15 V), the capillary suction time (CST) and specific resistance to filtration (SRF) were decreased by 88% and 92%, respectively. Efficient sludge stabilization with E. coli colonies of less than 1000 MPN/g TS was achieved. Phosphorus of 99% was removed from the filtrate and successfully fixed in the sludge cake and on the electrode surface. The integration of electrochemical and hypochlorite oxidation could effectively degrade the tightly bound extracellular polymeric substances (TB-EPS) structure with a total organic carbon (TOC) reduction of 52%. Besides, the disintegration of microbial cell envelopes was also achieved, with a reduction of living cell fraction of 98%. Furthermore, system pH could be maintained at near neutral (7.45) and the conversion of Fe(II) to Fe(III) was also facilitated with the addition of Ca(ClO)2, resulting in improved electrocoagulation process for enhanced sludge dewatering and phosphorus fixation. The multifunctional effects were achieved with the cooperated extracellular electrooxidation for EPS destruction and the active chlorine for intracellular microbial cell disintegration. This research provides a promising strategy for integrated sludge treatment and recycling for possible land utilization.

Although polyhalogenated carbazoles (PHCZs) can be generated and detected in drinking water, their occurrence and potential health risks to humans via drinking water ingestion are not well known. In this study, 11 PHCZs were screened in drinking water samples from Wuhan, the most populous city in central China. The total concentration of PHCZs could be up to 53.48 ng/L with a median level of 8.19 ng/L, which was comparable to polychlorinated biphenyls and poly- and perfluoroalkyl substances reported in the literatures for drinking water. Composition profiles revealed that 3,6-dichlorocarbazole, 3-chlorocarbazole, 3-bromocarbazole and 3,6-dibromocarbazole were the predominant PHCZ congeners in the tested samples. Regional differences in the levels and patterns of PHCZs suggested that anthropogenic releases should be the dominant source compared to natural generation. Boiling of the water samples caused no significant change in PHCZs concentrations after correcting the volume change due to evaporation. Potential health risks associated to the levels of PHCZs in drinking water were assessed using the toxic equivalent (TEQs) method. The estimated daily intake of PHCZs via drinking water ingestion is up to 0.38 pg-TEQ/kg body weight/day for infants, nearly 4.5 times higher than that for adults, and appears to reach the maximum permissible concentration set by certain authority agencies. Overall, drinking water ingestion represents an important exposure pathway for PHCZs. This is the first comprehensive study on the abundance and health risks of PHCZs in drinking water.

Sludge samples taken from different sources and times may have different characteristics that could affect dewatering performance. In this study, 20 sludge samples from five wastewater treatment plants and different seasons in 1 year were characterized. Pearson correlation analysis indicated that solid content (SC), total suspended solid (TSS), polysaccharides and proteins contents had positive correlations with the capillary suction time (CST), whereas volatile suspended–solid/total suspended solid (VSS/TSS) exhibited negative correlations with CST. Moreover, no correlations between CST and specific resistance to filtration were found among these different sludge samples. The principal component analysis confirmed that only two group variables could represent most of the sludge characteristic parameters. The first set of variables represents the particulate nature of the biotic factors (SC, VSS/TSS, SCOD, TSS, polysaccharides and proteins), and the second set is the pH. CST could not be a reasonable indicator of dewaterability in sludge deep dewatering by Fe2+/S2O8 2−-phosphogypsum composite conditioning. Furthermore, the results of diaphragm filter press dewatering showed that initial SC and VSS/TSS were the most dominant sludge characteristics affecting the solid content of dewatered cake (R p = 0.610, p = 0.016; R p = −0.838, p = 0.000, respectively) with Fe2+/S2O8 2−-phosphogypsum composite conditioning. Results from this study suggest that dewatering performance is predictable by sludge characteristics parameters for Fe2+/S2O8 2−-phosphogypsum conditioning.

Reuse of sludge-derived Fe-rich biochar as sludge conditioner is an attractive route for management of waste activated sludge at source. Homogeneous and heterogeneous Fenton reactions have been proved in sludge conditioning with Fe-rich biochar activating H2O2 to enhance sludge dewaterability. The FeAl2O4 phase in Fe-rich biochar was first identified during pyrolysis of sewage sludge after adding both Fe2O3 and Al2O3, since Fe and Al elements are two of major metal elements in Fe-rich sludge. Compared with the Fe-rich biochar that did not comprise FeAl2O4 phase, the capillary suction time (CST) and specific resistance to filterability (SRF) of the sludge conditioned with the Fe-rich biochar comprising FeAl2O4 phase could be efficiently decreased by 23% and 44%, respectively. The results indicated that FeAl2O4 phase in Fe-rich biochar could improve sludge dewaterability by enhancing heterogeneous Fenton reaction. Synergistic effect between Fe and Al in FeAl2O4 contributed to weak the O-O bond in H2O2 and reduce the activation energy of H2O2 decomposition for enhancing ·OH generation, which could be explained by density functional theory (DFT) calculations for the first time. Thus, the decomposition rate of H2O2 and the amount of ·OH generation were obviously promoted by FeAl2O4 phase in sludge-derived biochar during sludge conditioning, attributing to the destruction of sludge flocs, the release of bound water, and the improvement of sludge dewaterability.

An innovative cathodic algal biofilm microbial fuel cell equipped with a bioactive oxygen consuming unit (AB-OCU-MFC) was proposed for enhancing the leachate treatment containing biorefractory organic matters and high strength of ammonium nitrogen. The proposed AB-OCU-MFC performed better with regard to COD, NH4+-N, TN removals and algal biomass yield than standalone algal biofilm-MFC and control reactors. AB-OCU-MFC with OCU of 2 cm thickness removed more than 86% of COD, 89.4% of NH4+-N, 76.7% of TN and produced a maximum voltage of 0.39 V and biomass productivity of 1.23 g·L−1·d−1. The High-throughput sequencing of DNA showed a significant change in microbial community of reactors implemented with OCU, in which the ratio of exoelectrogenic bacteria of anode and denitrifying bacteria on cathode were significantly increased. The results obtained by cathodic algal biofilm MFC with low cost and bioactive barrier of OCU, would provide a new sight for practical application of MFC.

Fe-rich biochar with multivalent iron compounds (Fe0, Fe0.95C0.05, Fe3O4, and FeAl2O4) pyrolyzed from sludge cake conditioned with Fenton's reagent and red mud was utilized as an efficient Fenton catalyst for the degradation of 4-chlorophenol (4-CP). Effects of pyrolysis temperature and sludge conditioner composition on the transformation of iron compounds were studied. Both homogeneous Fenton reaction initiated by Fe2+ leached from both low-valent Fe0 and Fe0.95C0.05, and heterogeneous Fenton reaction initiated by solid iron phases of Fe3O4 and FeAl2O4 were revealed to contribute to the degradation of 4-CP. The removal efficiency of 4-CP remained 100% after five successive degradation rounds. The homogeneous Fenton reaction mainly works in the first degradation round, and the heterogeneous Fenton reaction dominates in subsequent degradation rounds. The findings of this study suggest that sewage sludge derived Fe-rich biochar could be utilized as an efficient Fenton catalyst for recalcitrant organics degradation.

The novel catalyst LaCu0.5Fe0.5O3-δ with oxygen vacancies (OVs) was prepared and demonstrated excellent stability and activity for the degradation of bisphenol A. The removal rate of 92.1 % and H2O2 utilization efficiency of 70.4 % were obtained due to the efficient hydroxyl radical generation mediated by OVs. The density functional theory calculation showed that the substitution of Cu and formation of OVs significantly increases the charge density near the active sites. Bader charge analysis revealed that the charge offset accelerated the reduction of Fe. The elevation of electron transfer efficiency also promotes the valence transition of copper and iron atoms. The reversible electronic transition between Fe2+ ⇆ Fe3+, Cu+ ⇆ Cu2+ and Cu2+ ⇆ Fe2+ involved in this reaction were considered to be enhanced and the homolytic bond clearage of H2O2 was simultaneously promoted, facilitated by the electron-rich region combined with OVs on the surface of LaCu0.5Fe0.5O3-δ.

A coupled microbial electrolysis cell - anaerobic granular sludge system (MEC-AGS) was established to explore the degradation efficiency of 2,4,6-trichlorophenol (TCP) with synchronous biogas production. Results showed that MEC-AGS yielded a higher proportion of CH4 than MEC (83.8 ± 0.4% vs 82.0 ± 1.0%, P

A novel technique for phosphorus recovery from the liquid phase of anaerobic digestate was developed using biochar derived from iron−rich sludge (dewatered sludge conditioned with Fenton’s reagent). The biochar pyrolyzed from iron−rich sludge at a low temperature of 300 °C (referred to as Fe−300 biochar) showed a better phosphorus (P) adsorption capacity (most of orthophosphate and pyrophosphate) than biochars pyrolyzed at other higher temperatures of 500–900 °C, with the maximum P adsorption capacity of up to 1.843 mg g−1 for the liquid phase of anaerobic digestate. Adsorption isotherms study indicated that 70% P was precipitated through chemical reaction with Fe elements, i.e., Fe(II) and Fe(III) existed on the surface of the Fe−300 biochar, and other 30% was through surface physical adsorption as simulated by a dual Langmuir-Langmuir model using the potassium dihydrogen orthophosphate (KH2PO4) as a model solution. The seed germination rate was increased up to 92% with the addition of Fe−300 biochar after adsorbing most of P, compared with 66% without the addition of biochar. Moreover, P adsorbed by the chemical reaction in form of iron hydrogen phosphate can be solubilized by a phosphate-solubilizing microorganism of Pseudomonas aeruginosa, with the total solubilized P amount of 3.045 mg g−1 at the end of an incubation of 20 days. This study indicated that the iron−rich sludge−derived biochar could be used as a novel and beneficial functional material for P recovery from the liquid phase of anaerobic digestate. The recovered P with biochar can be re-utilized in garden soil as an efficient P−fertilizer, thus increasing the added values of both the liquid phase of anaerobic digestate and the iron−rich sludge.

Suspended solids (SS) are one of major pollutants that deteriorate water quality. The high-rate clarifier is commonly used as the tertiary treatment by coagulation to agglomerate particles, thus achieving a high SS removal and making effluents acceptable for discharge. Currently the control of average residence time in operation of high-rate clarifier is challenging: With limited residence time, the particles fail to form flocs in the mixing tank, causing inefficient solid/liquid separation; while with prolonged residence time, SS sedimentation would accumulate at the bottom of the tank. In this study, a liquid-solid two-phase computational fluid dynamics (CFD) model has been developed to simulate the distributions of flow field and SS in a high-rate clarifier. The CFD model was successfully validated against experimental results in a full-scale operation, with the normalized standard error on SS less than 1.24 %. The results showed that the height of under-through channel affected the flow field more significantly rather than its width. This study also indicated that with the height of under-through channel decreasing from 2000 to 500 mm and the height of baffle increasing from 3300 to 5213 mm, the average SS concentration at the bottom of reaction tank would decrease by 34.95 % and the average residence time would be shortened by 4.77 %, which can be helpful for prolonging dredging cycle and avoiding unnecessary dredging costs.

A facile one-pot solvothermal method was applied to synthesize a magnetic biochar composite (MB) using phoenix tree leaves-derived biochar as the carbon matrix. The structure of MB was optimized by varying the load ratio and particle size of Fe3O4 nanoparticles on biochar. Time-dependent structure and composition evolution of solid and liquid phases during heterogeneous solvothermal process were investigated to understand the formation mechanism of MB. Firstly, Fe2+/Fe3+ ions were coordinated by oxygen-containing groups on biochar and part of them were hydrolyzed to form iron hydroxides. Then, those iron-containing precursors were thermally decomposed and reduced to iron oxides; and finally Fe3O4 nanoparticles were generated. The MB had an adsorption capacity for Cr(VI) of 55.0 mg/g in an aqueous solution, which exceeds those of biochar (39.8 mg/g) and Fe3O4 nanoparticles (26.5 mg/g). The adsorption mechanism study reveals that biochar as a carbon skeleton mainly provided binding sites for Cr(VI) and electron-donor groups for reduction of Cr(VI), while Fe3O4 nanoparticles mainly involved in the immobilization of newly formed Cr(III) through formation of Fe(III)-Cr(III) hydroxide. MB exhibited a stable structure with a lower Fe leakage at pH 2.0 than that of a comparable magnetic biochar sample prepared by conventional co-precipitation method. Recycling experiments suggested that MB could keep 84% of its initial removal capability for Cr(VI) even after seven cycles. The results indicate that solvothermal method is a promising alternative to prepare magnetic biochar for adsorption of heavy metal-containing wastewater.

Fenton's reagent has been widely used to enhance sludge dewaterability. However, drawbacks associated with hydrogen peroxide (H2O2) in Fenton's reagents exist, since it is a hazardous chemical and shows carcinogenicity, explosivity, instability, and corrosivity. Moreover, initial acidification and subsequent neutralization are needed as optimal conditions for homogeneous Fenton conditioning and final filtrate discharge. In this study, a Fenton-like process for the enhanced dewaterability of waste activated sludge with in-situ generation of H2O2 and without extra pH adjustment was firstly proposed, namely citric acid (CA)-assisted oxygen activation in an air/nano zero-valent iron (nZVI) system and chemical re-coagulation with polydiallyldimethylammonium chloride (PDMDAAC). Using the response surface methodology (RSM), the optimal doses of CA, nZVI, and PDMDAAC were determined to be 13, 33, and 9 mg g−1 dry solids (DS), respectively. This composite conditioner showed a good dewatering capability compared with the raw sludge, e.g. the capillary suction time decreased from 130.0 to 9.5 s. The enhanced sludge dewaterability was further confirmed by laboratory-scale diaphragm filter press dewatering tests, which produced a lower cake moisture content compared with the raw sludge, and the final pH of the filtrate was close to neutrality. The citric acid promoted the production of H2O2 and Fe(II)/Fe(III) species, the degradation of protein in tightly-bound extracellular polymeric substances, and the decomposition of protein-N in the solid phase of sludge, resulting a greater conversion of bound water to free water. The results of electron spin resonance indicated that the hydroxyl radicals were mainly responsible for the decomposition of proteinaceous compounds. The subsequent chemical re-coagulation with PDMDAAC can make the zeta potential of sludge samples less negative, reduce the repulsive electrostatic interactions, and agglomerate the smaller particles into larger aggregates, thus enhancing sludge dewaterability.