Thermodynamic Inhibition of Microbial Sulfur Disproportionation in a Multisubunit Designed Sulfur-Siderite Packed Bioreactor.

Sulfur disproportionation (S0DP) poses a challenge to the robust application of sulfur autotrophic denitrification due to unpredictable sulfide production, which risks the safety of downstream ecosystems. This study explored the S0DP occurrence boundaries with nitrate loading and temperature effects. The boundary values increased with the increase in temperature, exhibiting below 0.15 and 0.53 kg-N/m3/d of nitrate loading at 20 and 30 °C, respectively. A pilot-scale sulfur-siderite packed bioreactor (150 m3/d treatment capacity) was optimally designed with multiple subunits to dynamically distribute the loading of sulfur-heterologous electron acceptors. Operating two active and one standby subunit achieved an effective denitrification rate of 0.31 kg-N/m3/d at 20 °C. For the standby subunit, involving oxygen by aeration effectively transformed the facultative S0DP functional community from S0DP metabolism to aerobic respiration, but with enormous sulfur consumption resulting in ongoing sulfate production of over 3000 mg/L. Meanwhile, acidification by the sulfur oxidation process could reduce the pH to as low as 2.5, which evaluated the Gibbs free energy (ΔG) of the S0DP reaction to +2.56 kJ, thermodynamically suppressing the S0DP occurrence. Therefore, a multisubunit design along with S0DP inhibition strategies of short-term aeration and long-term acidification is suggested for managing S0DP in various practical sulfur-packed bioreactors.

Highly Efficient Coremoval of Nitrate and Phosphate Driven by a Sulfur-Siderite Composite Reactive Filler toward Secondary Effluent Polishing.

Reactive fillers consisting of reduced sulfur and iron species (SFe-ReFs) have received increasing attention in tertiary wastewater treatment for nitrate and phosphate coremoval. However, the existing SFe-ReFs suffer from either low performance (e.g., pyrrhotite and pyrite) or unsatisfactory use in terms of combustible risk and residual nonreactive impurities (e.g., sulfur mixing with natural iron ores). Here, we developed a new type of sulfur-siderite composite ReF (SSCReF) with a structure of natural siderite powders eventually embedded into sulfur. SSCReFs exhibited many excellent properties, including higher mechanical strengths and hardness and especially much poorer ignitability compared to pure sulfur. By using SSCReF to construct packed-bed reactors, the highest denitrification and dephosphorization rates reached 829.70 gN/m3/d (25 wt % siderite) and 36.70 gP/m3/d (75 wt % siderite), respectively. Dephosphorization was demonstrated to be dependent on sulfur-driven denitrification, in which the acid produced from the later process promoted Fe(II) dissolution, which then directly combined with phosphate to form vivianite or further converted into phosphate adsorbents (ferrihydrite, a green rust-like compound). Water flush was an effective way to finally wash out these surface deposited Fe-P compounds, as well as those nonreactive impurities (Si and Al-bearing compounds) detached from SSCReF. Such a highly efficient and safe SSCReF holds considerable application potential in secondary effluent polishing.

Response of sulfur-metabolizing biofilm to external sulfide in element sulfur-based denitrification packed-bed reactor.

Dosing sulfide into the sulfur-packed-bed (S0PB) has great potential to enhance the denitrification efficiency by providing compensatory electron donors, however, the response of sulfur-metabolizing biofilm to various sulfide dosages has never been investigated. In this study, the S0PB reactor was carried out with increasing sulfide dosages by 3.6 kg/m3/d, presenting a decreasing effluent nitrate from 14.2 to 2.7 mg N/L with accelerated denitrification efficiency (k: 0.04 to 0.27). However, 6.5 mg N/L of nitrite accumulated when the sulfide dosage exceeded 0.9 kg/m3/d (optimum value). The increasing electron export contribution of sulfide a maximum of 85.5% illustrated its competition with the in-situ sulfur. Meanwhile, over-dosing sulfide caused serious biofilm expulsion with significant decreases in the total biomass, live cell population, and ATP by 90.2%, 86.7%, and 54.8%, respectively. This study verified the capacity of dosing sulfide to improve the denitrification efficiency in S0PB but alerted the negative effect of exceeded dosing.

Synergistic between autotrophic and heterotrophic microorganisms for denitrification using bio-S as electron donor.

In recent years, biological sulfur (bio-S) was employed in sulfur autotrophic denitrification (SAD) in which autotrophic Thiobacillus denitrificans and heterotrophic Stenotrophomonas maltophilia played a key role. The growth pattern of T.denitrificans and S.maltophilia exhibited a linear relationship between OD600 and CFU when OD600 < 0.06 and <0.1, respectively. When S.maltophilia has applied alone, the NorBC and NosZ were undetected, and denitrification was incomplete. The DsrA of S.maltophilia could produce sulfide as an alternative electron donor for T.denitrificans. Even though T.denitrificans had complete denitrification genes, its efficiency was low when used alone. The interaction of T.denitrificans and S.maltophilia reduced nitrite accumulation, leading to complete denitrification. A sufficient quantity of S.maltophilia may trigger the autotrophic denitrification activity of T.denitrificans. When the colony-forming units (CFU) ratio of S.maltophilia to T.denitrificans was reached at 2:1, the highest denitrification performance was achieved at 2.56 and 12.59 times higher than applied alone. This research provides a good understanding of the optimal microbial matching for the future application of bio-S.

Insight into the shaping of microbial communities in element sulfur-based denitrification at different temperatures.

Nitrate pollution is an important cause of eutrophication and ecological disruption. Recently, element sulfur-based denitrification (ESDeN) has attracted increasing attention because of its non-carbon source dependence, low sludge yield, and cost-effectiveness. Although the denitrification performance of sulfur autotrophic denitrifying bacteria at different temperatures has been widely studied, there are still many unknown factors about the adaptability and the shaping of microbial community. In this study, we comprehensively understood the shaping of ESDeN microbial communities under different temperature conditions. Results revealed that microbial communities cultivated at temperatures ranging from 10 °C to 35 °C could be classified as high-temperature (35 °C), middle-temperature (30, 25 and 20 °C), and low-temperature (15 and 10 °C) communities. Dissolved oxygen in water was an important factor that, in combination with temperature, shaped microbial community structure. According to network analysis, the composition of keystone taxa was different for the three groups of communities. Some bacteria that did not have sulfur compound oxidation function were identified as the "keystone species". The abundances of carbon, nitrogen, and sulfur metabolism of the three microbial communities were significantly changed, which was reflected in that the high-temperature and middle-temperature communities were dominated by dark oxidation of sulfur compounds and dark sulfide oxidation, while the low-temperature community was dominated by chemoheterotrophy and aerobic chemoheterotrophy. The fact that the number of microorganisms with dark oxidation of sulfur compounds capacity was quite higher than that of microorganisms with dark sulfur oxidation capacity suggested that the sulfur bioavailability at different temperatures, especially low temperature, was the main challenge for the development of efficient ESDeN process. This study provided a biological basis for developing a high-efficiency ESDeN process to cope with temperature changes in different seasons or regions.

Thiosulfate as external electron donor accelerating denitrification at low temperature condition in S0-based autotrophic denitrification biofilter.

This study was carried out to determine the inhibition of low temperature on the performance of S0-based autotrophic denitrification (S0-SAD) biofilter, and proposed to enhance the nitrate removal efficiency with thiosulfate as external electron donor. With the decline of temperature from 30 °C to 10 °C at 0.25 h of empty bed contact time (EBCT), the nitrate removal rate presented a logarithmical drop, and the effluent nitrate dramatically increased from 9.19 mg L-1 to 15.13 mg L-1. EBCT was prolonged until 0.33 h for 20 °C, 0.66 h for 15 °C and 1.5 h for 10 °C, respectively, to maintain the effluent nitrate below 10 mg L-1. Such excessive variation of EBCT for different temperature is undoubtedly incredible for practical engineering. Thiosulfate, as the external electron donor, was adopted to compensate the efficiency loss during temperature decrease, which significantly prompted nitrate removal rate to 0.59, 0.53 and 0.31 kg N m-3 d-1 at 20 °C, 15 °C and 10 °C conditions, respectively, even at a short EBCT of 0.25 h. It not only acted as compensatory electron donor for nitrate removal, but also promoted the contribution of elemental sulfur via accelerating the DO consumption and extended larger effective volume of S0-layer for denitrification. Meanwhile, the significant enrichment of Sulfurimonas and Ferritrophicum provided biological evidences to the enhancement process. However, the incomplete consumption of thiosulfate was observed especially at EBCT of 0.25 h and 10 °C, and the thiosulfate runoff needs to be concerned in case of contaminating the effluent. Herein, approximately extending EBCT to 0.66 h and decreasing thiosulfate dosage were conducted simultaneously, thereby achieving 100% thiosulfate utilization efficiency and expected nitrate removal. This study provided a fundamental guidance to design and operate S0-SAD biofilter in response to seasonal temperature variation for practical engineering.

Mitigating nitrite accumulation during S0-based autotrophic denitrification: Balancing nitrate-nitrite reduction rate with thiosulfate as external electron donor.

This study was carried out to determine the effect of influent nitrate loading on nitrite accumulation during elemental-sulfur based denitrification process, and proposed to enhance the nitrogen removal efficiency by mitigating nitrite accumulation with thiosulfate as external electron donor. Along with increasing the nitrate influent loading (from 0.09 kg N/m3/d to 1.73 kg N/m3/d) by shortening the empty bed contact time (EBCT) (from 5 h to 0.25 h), the nitrate removal loading increased from 0.08 to 0.83 kg N/m3/d. Meanwhile, the raise of the nitrate influent loading obviously aggravated the nitrite accumulation. Herein, nitrite began to accumulate since the nitrate influent loading was over 0.86 kg N/m3/d, and a maximum nitrite accumulation of 2.39 mg/L was observed under the 0.25 h of EBCT and 15 mg/L of nitrate influent concentration condition. Thiosulfate was used as the external electron donor to accelerate the nitrite reduction rate in order to mitigate the nitrite accumulation. As a result, the nitrite accumulation significantly decreased from 2.39 mg/L to 0.17 mg/L with the thiosulfate dosage of 13.36 mg/L. However, the nitrite accumulation bounced with the on-going increase of the thiosulfate dosage, indicating that the nitrate reduction rate and nitrite reduction rate were accelerated alternatively. After dosing thiosulfate, the relative abundances of sulfurimonas and ferritrophicum grew up significantly.

Sulfur autotrophic denitrification filter and heterotrophic denitrification filter: Comparison on denitrification performance, hydrodynamic characteristics and operating cost.

Sulfur autotrophic denitrification (SAD) process, as an alternative to heterotrophic denitrification (HD) filter, receives growing interest in polishing the effluent from secondary sewage treatment. Although individual studies have indicated several advantages of SAD over HD, rare study has compared these two systems under identical condition and by using real secondary effluent. In this study, two small pilot scale filters (SAD and HD) were designed with identical configuration and operated parallelly by feeding the real secondary effluent from a WWTP. The results showed SAD filter can be started up without the addition of soluble electron donor, although the time (14 days) was about 3 times longer than that of HD filter. The nitrate removal rate of SAD filter at HRT of 1.4 h was measured as 0.268 ± 0.047 kg N/(m3∙d). Similar value was observed in HD filter with supplementing 90 mg/L COD. The COD concentration of effluent always kept lower than that of influent in SAD filter but not in HD filter. In addition, SAD filter could maintain a stable denitrification performance without backwash for 15 days, while decline of nitrate removal rate was observed in HD filter just 2 days after stopping the backwash. This different behavior was further confirmed as the SAD filter had a better hydraulic flow pattern. Analysis according to high-throughput 16S rRNA gene-based Illumina MiSeq sequencing clearly showed the microbial community evolution and differentiation among the samples of seed sludge, SAD and HD filters. Finally, the economic assessment was carried out, showing the operation cost of SAD filter was over 50% lower than that of HD filter.

Wire-drawing process with graphite lubricant as an industrializable approach to prepare graphite coated stainless-steel anode for bioelectrochemical systems.

Carbon coated stainless-steel (SS) electrode has been suggested to be a powerful composite electrode with high conductivity, excellent biocompatibility and good mechanical strength, which is promising for scaling up the bioelectrochemical systems (BESs). However, the already reported carbon coating methods were independent on the production of SS material. Additional steps and investment of equipment for carbon coating are costly, and the industrialization of these carbon coating processes remains challenging. In this study, we report an industrializable carbon coating approach that was embedded into the production line of the SS wire, which was realized through a wire-drawing process with graphite emulsion as the lubricant and carbon source. We found the slide of SS wire through the dies was essential for the graphite coating in terms of loading amount and stability. When the graphite coated SS wire was prepared as the anode and operated in a BESs, the current density reached 1.761 ± 0.231 mA cm-2, which was 20 times higher than that without graphite coating. Biomass analysis was then conducted, confirming the superior bioelectrochemical performance was attributed to the improvement of biocompatibility by the graphite coating layer. Furthermore, graphite coating by the wire-drawing process was systematically compared with the existing methods, which showed a comparable or even better bioelectrochemical performance but with extremely low cost (0.036 $·m-2) and seconds level of the time consumption. Overall, this study offers a cost-effective and industrializable approach to preparing graphite coated SS electrode, which may open up great opportunities to promote the development of BESs at large scale.

Insights into palladium nanoparticles produced by Shewanella oneidensis MR-1: Roles of NADH dehydrogenases and hydrogenases.

Biologically synthesized palladium nanoparticles (bio-Pd) have attracted considerable interest as promising green catalysts for environmental remediation. However, the mechanisms by which microorganisms produce bio-Pd remain unclear. In the present study, we investigated the roles of Shewanella oneidensis MR-1 and its NADH dehydrogenases and hydrogenases (HydA and HyaB) in bio-Pd production using formate as the electron donor. The roles of NADH dehydrogenases and hydrogenases were studied by inhibiting NADH dehydrogenases and using hydrogenase mutants (ΔhydA, ΔhyaB, and ΔhydAΔhyaB), respectively. The results showed ~97% reduction of palladium by S. oneidensis MR-1 after 24 h using 250 µM palladium and 500 µM formate. Electron microscopy images showed the presence of bio-Pd on both the outer and cytoplasmic membranes of S. oneidensis MR-1. However, the inhibition of NADH dehydrogenases in S. oneidensis MR-1 resulted in only ~61% reduction of palladium after 24 h, and bio-Pd were not found on the outer membrane. The mutants lacking one or two hydrogenases removed 91-96% of palladium ions after 24 h and showed more cytoplasmic bio-Pd but less periplasmic bio-Pd. To the best of our knowledge, this is the first study to demonstrate the role of NADH dehydrogenases of S. oneidensis MR-1 in the formation of bio-Pd on the outer membrane. It also demonstrates that the hydrogenases (especially HyaB) of S. oneidensis MR-1 contribute to the formation of bio-Pd in the periplasmic space. This study provides mechanistic insights into the production of biogenic metal nanoparticles towards their possible use in industrial and environmental applications.

Perylene pigment wastewater treatment by fenton-enhanced biological process.

Polycyclic aromatic hydrocarbons (PAHs) are regarded as priority pollutants owing to their toxic, mutagenic and carcinogenic characteristics. Perylene is a kind of 5-ring PAH with biological toxicity, and classified as a class III carcinogen by the World Health Organization (WHO). Nowadays, some of its derivatives are often used as industrial pigments. Hence, urgent attention is highly needed to develop new and improved techniques for PAHs and their derivatives removal from the environment. In this study, Fenton oxidation process was hybridized with the biological (anaerobic and aerobic) treatments for the removal of perylene pigment from wastewater. The experiments were carried out by setting Fenton treatment system before and between the biological treatments. The biological results showed that COD removal efficiency reached 60% during 24 h HRT with an effluent COD concentration of 1567.78 mg/L. After the HRT increased to 48 h, the COD removal efficiency was slightly increased (67.9%). However, after combining Fenton treatment with biological treatment (Anaerobic-Fenton-Aerobic), the results revealed over 85% COD removal efficiency and the effluent concentration less than 600 mg/L which was selected as the better treatment configuration for the biological and chemical combined system. The microbial community analysis of activated sludge was carried out with high-throughput Illumina sequencing platform and results showed that Pseudomonas, Citrobacter and Methylocapsa were found to be the dominant genera detected in aerobic and anaerobic reactors. These dominant bacteria depicted that the community composition of the reactors for treating perylene pigments wastewater were similar to that of the soil contaminated by PAHs and the activated sludge from treating PAHs wastewater. Economic analysis results revealed that the reagent cost was relatively cheap, amounting to 10.64 yuan per kilogram COD. This study vividly demonstrated that combining Fenton treatment with biological treatment was efficient and cost-effective.

Shewanella oneidensis MR-1 self-assembled Pd-cells-rGO conductive composite for enhancing electrocatalysis.

Biosynthesized noble metal nanoparticles (NPs) as promising green catalysts for electrochemical application has invited a lot of attention. However, effective electron transfer between biosynthesized NPs and electrode remains a challenge due to the uncontrollable and poor conductive property of cell substrates. In this study, graphene oxide (GO) was introduced into a bio-Pd synthesis process governed by Shewanella oneidensis MR-1, which was demonstrated to be simultaneously reduced with Pd(II) and transformed to reduced GO (rGO), resulting in the formation of a Pd-cells-rGO composite. Compared to the control without rGO (Pd-cells), the electrochemical conductivity of Pd-cells-rGO composite increased from almost zero to 196 µS cm-1, indicating the rGO facilities the electron transport across the composite. Electrochemical characterizations revealed the electrochemical active surface area (ECSA) of Pd in Pd-cells-rGO was enlarged by increasing the amount of rGO in the composite, clearly indicating that the conductive network created by rGO enable the Pd NPs receive electrons from electrode and become electrochemical active. A considerable enhancement of electrocatalytic activity was further confirmed for Pd-cells-rGO as indicated by 36.7- and 17.2-fold increase (Pd-cells-rGO with Pd/GO ratio of 5/1 vs Pd-cells) of steady state current density toward hydrogen evolution and nitrobenzene reduction at -0.7 V and -0.55 V vs Ag/AgCl, respectively. We also compared the electrocatalytic performance with MWCNTs hybrids Pd-cells-CNTs. It was found that the association of Pd, cells and rGO creates an interactive and synergistic environment to allow higher conductivity and catalytic activity under the same amount of carbon nanomaterial. The strategy developed in this work activates a highly reactive NPs and proposed a designable protocol for enhancing electrocatalytic activity of biocatalysts.

NO Removal with Efficient Recovery of N2O by Using Recyclable Fe3O4@EDTA@Fe(II) Complex: A Novel Approach toward Resource Recovery from Flue Gas.

Traditional technologies for handling nitrogen oxides (NO x) from flue gas commonly entail the formation of harmless nitrogen gas (N2), while less effort has been made to recover the N-containing chemicals produced. In this work, we developed a novel nanomagnetic adsorbent, Fe3O4@EDTA@Fe(II) (MEFe(II)), for NO removal. The NO adsorbed by MEFe(II) was then selectively converted to N2O, a valuable compound in many industries, by using sulfite (a product from desulfurization in flue gas treatment) as the reductant for the regeneration of MEFe(II). Because of the magnetic and solid properties of MEFe(II), the processes of NO adsorption and N2O recovery can be readily carried out under their optimal pH conditions in separate systems. In addition, the produced N2O is easily handled without unwanted release to the atmosphere. At the optimal pH (7.5 and 8.0 for NO adsorption and N2O recovery, respectively), the maximum NO adsorption capacity of MEFe(II) was measured as 0.303 ± 0.037 mmol·g-1, over 90% of which was converted to N2O during the recovery process. Moreover, MEFe(II) exhibited good five consecutive cycles. All of above reactions were performed at room temperature. These findings indicate MEFe(II) may hold great potential for application to NO removal from flue gas with the benefits of resource recovery, decreased chemical use, and low energy consumption.

Coupled Sulfur and Iron(II) Carbonate-Driven Autotrophic Denitrification for Significantly Enhanced Nitrate Removal.

Sulfur-based denitrification process has attracted increasing attentions because it does not rely on the external addition of organics and avoids the risk of COD exceeding the limit. Traditionally, limestone is commonly employed to maintain a neutral condition (SLAD process), but it may reduce the efficiency as the occupied zone by limestone cannot directly contribute to the denitrification. In this study, we propose a novel sulfur-based denitrification process by coupling with iron(II) carbonate ore (SICAD system). The ore was demonstrated to play roles as the buffer agent and additional electron donor. Moreover, the acid produced through sulfur driven denitrification was found to promote the Fe(II) leaching from the ore and likely extend the reaction zone from the surface to the liquid. As a result, more biomass was accumulated in the SICAD system compared with the controls (sulfur, iron(II) carbonate ore and SLAD systems). Owing to these synergistic effects of sulfur and iron(II) carbonate on denitrification, SICAD system showed much higher denitrification rate (up to 720.35 g·N/m3·d) and less accumulation of intermediates (NO2- and N2O) than the controls. Additionally, sulfate production in SICAD system was reduced. These findings offer great potential of SICAD system for practical use as a highly efficient postdenitrification process.

Borate Inorganic Cross-Linked Durable Graphene Oxide Membrane Preparation and Membrane Fouling Control.

Graphene oxide (GO) membranes have the potential to be next-generation membranes. However, the GO layer easily swells in water and risks shedding during the long-term filtration. Organic GO interlayer organic cross-linking agent was not resistant to oxidation, which limits the application scope of GO membrane. In this study, an inorganic cross-linked GO membrane was prepared via the reaction of sodium tetraborate and GO hydroxyl groups, and a -B-O-C- cross-linking bond was detected by X-ray photoelectron spectroscopy (XPS). Additionally, a new atomic force microscope scratch method to evaluate the cross-linking force of a nanoscale GO layer was proposed. It showed that the critical destructive load of the inorganic cross-linked GO membrane increased from 8 to 80 nN, which was a 10-fold increase from that of the nonlinked sample. During the NaOH/sodium dodecyl sulfate (SDS) destructive wash tests, morphology, flux and retention rate of inorganic cross-linked GO remained stable while the comparative membranes showed significant destruction. At the same time, based on the better oxidation resistance, organic membrane fouling was effectively controlled by the introduction of trace ·OH radicals. This study provides a new perspective for GO membrane preparation, interlayer cross-linking force testing and membrane fouling control.

Microbial Photoelectrotrophic Denitrification as a Sustainable and Efficient Way for Reducing Nitrate to Nitrogen.

Biological removal of nitrate, a highly concerning contaminant, is limited when the aqueous environment lacks bioavailable electron donors. In this study, we demonstrated, for the first time, that bacteria can directly use the electrons originated from the photoelectrochemical process to carry out the denitrification. In such photoelectrotrophic denitrification (PEDeN) systems (denitrification biocathode coupling with TiO2 photoanode), nitrogen removal was verified solely relying on the illumination dosing without consuming additional chemical reductant or electric power. Under the UV illumination (30 mW·cm-2, wavelength at 380 ± 20 nm), nitrate reduction in PEDeN apparently followed the first-order kinetics with a constant of 0.13 ± 0.023 h-1. Nitrate was found to be almost completely converted to nitrogen gas at the end of batch test. Compared to the electrotrophic denitrification systems driven by organics (OEDeN, biocathode/acetate consuming bioanode) or electricity (EEDeN, biocathode/abiotic anode), the denitrification rate in PEDeN equaled that in OEDeN with a COD/N ratio of 9.0 or that in EEDeN with an applied voltage at 2.0 V. This study provides a sustainable technical approach for eliminating nitrate from water. PEDeN as a novel microbial metabolism may shed further light onto the role of sunlight played in the nitrogen cycling in certain semiconductive and conductive minerals-enriched aqueous environment.

Efficient treatment of azo dye containing wastewater in a hybrid acidogenic bioreactor stimulated by biocatalyzed electrolysis.

In this study, a novel scaled-up hybrid acidogenic bioreactor (HAB) was designed and adopted to evaluate the performance of azo dye (acid red G, ARG) containing wastewater treatment. Principally, HAB is an acidogenic bioreactor coupled with a biocatalyzed electrolysis module. The effects of hydraulic retention time (HRT) and ARG loading rate on the performance of HAB were investigated. In addition, the influent was switched from synthetic wastewater to domestic wastewater to examine the key parameters for the application of HAB. The results showed that the introduction of the biocatalyzed electrolysis module could enhance anoxic decolorization and COD (chemical oxygen demand) removal. The combined process of HAB-CASS presented superior performance compared to a control system without biocatalyzed electrolysis (AB-CASS). When the influent was switched to domestic wastewater, with an environment having more balanced nutrients and diverse organic matters, the ARG, COD and nitrogen removal efficiencies of HAB-CASS were further improved, reaching 73.3%±2.5%, 86.2%±3.8% and 93.5%±1.6% at HRT of 6 hr, respectively, which were much higher than those of AB-CASS (61.1%±4.7%, 75.4%±5.0% and 82.1%±2.1%, respectively). Moreover, larger TCV/TV (total cathode volume/total volume) for HAB led to higher current and ARG removal. The ARG removal efficiency and current at TCV/TV of 0.15 were 39.2%±3.7% and 28.30±1.48 mA, respectively. They were significantly increased to 62.1%±2.0% and 34.55±0.83 mA at TCV/TV of 0.25. These results show that HAB system could be used to effectively treat real wastewater.

Inducement mechanism and control of self-acidification in elemental sulfur fluidizing bioreactor.

The sulfur fluidizing bioreactor (S0FB) has significant superiorities in treating nitrate-rich wastewater. However, substantial self-acidification has been observed in engineering applications, resulting in frequent start-up failures. In this study, self-acidification was reproduced in a lab-scale S0FB. It was demonstrated that self-acidification was mainly induced by sulfur disproportionation process, accounting for 93.4 % of proton generation. Supplying sufficient alkalinity to both the influent (3000 mg/L) and the bulk (2000 mg/L) of S0FB was essential for achieving a successful start-up. Furthermore, the S0FB reached 10.3 kg-N/m3/d of nitrogen removal rate and 0.13 kg-PO43-/m3/d of phosphate removal rate, respectively, surpassing those of the documented sulfur packing bioreactors by 7-129 times and 26-65 times. This study offers a feasible and practical method to avoid self-acidification during restart of S0FB and highlights the considerable potential of S0FB in the treatment of nitrate-rich wastewater.

Improved efficiency and stability using a novel elemental sulfur-based moving-bed denitrification process.

Elemental sulfur-based denitrification (ESDeN) technology is known as a cost-saving alternative to its heterotrophic counterpart for nutrient removal from organic-deficient water. However, the traditional fixed-bed reactor (FixBR), as an extensively used process, suffers from a low denitrification rate and even performance deterioration during long-term operation. Herein, we proposed a novel elemental sulfur-based denitrifying moving-bed reactor (ESDeN-MovBR), in which a screw rotator was employed to drive the filled sulfur particles to be microfluidized vertically (a state of vertical-loop movement). Our results showed that the ESDeN-MovBR realized much superior and more stable denitrification performance compared to the ESDeN-FixBR, as indicated by 3.09-fold higher denitrification rate and over one order of magnitude lower intermediates (NO2- and N2O) yield, which could last for over 100 days. Further research revealed that the microfluidization of sulfur particles facilitated the expelling of nitrogen bubbles and excessive biomass, resulting in the prolongation of actual hydraulic retention time by over 80 % and could partially explain the higher denitrification rate in ESDeN-MovBR. The remaining contribution to the improvement of denitrification rate was suggested to be result from changes in biofilm properties, in which the biofilm thickness of ESDeN-MovBR was found to be 3.29 times thinner yet enriched with 2.52 times more autotrophic denitrifiers. This study offered a completely new solution to boost up the denitrification performance of ESDeN technology and provided in-depth evidence for the necessity of biofilm thickness control in such technology.