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This study was carried out to determine the inhibition of low temperature on the performance of S

The effect of particle morphology on denitrification performance in element sulfur-based denitrification (ESDeN) packed-bed process is a gap. In this study, three different types of commercial sulfur particles were selected to build the ESDeN reactors. The results showed the reactors filled with rougher sulfur particles took shorter time to reach stable denitrification performance in the start-up stage. The reactors filled with cap-shape sulfur particles received the maximum nitrate removal rate of 849.49 ± 79.29 g N m

Economic options to retrofit wastewater treatment plants (WWTPs) without tertiary treatments need to be explored. In this regard, bioelectrochemical systems (BES) can be hybridized with existing technologies, upgrading the removal performance of original techniques while avoiding replacement costs. Yet, few demonstrations of merged systems have been given. For the first time, in this work it was built a lab-scale model of a BES merged with a secondary settler, namely e-settler, to enhance the polishing performance of already existing WWTPs. In particular, to concomitantly increase nitrogen removal and perform wastewater (WW) disinfection, avoiding further tertiary treatments. In the e-settlers, nitrogen removal was increased through bioelectrochemical stimulation. Concomitant ammonium and nitrate removal without nitrite accumulation and a negligible amount of nitrous oxide emissions were observed. Ti-MMO as anode material showed a high disinfectant action. In conclusion, it was demonstrated how a simple bioelectrochemical set-up can upgrade existing WWTPs. The following step requires the study at a larger scale, identifying optimal operational and structural parameters for the in-situ application. The main limitations of the e-settlers were discussed, linking them to possible solutions that need to be deepened in a lab-scale model of conventional secondary treatments (activated sludge followed by secondary settler) This work was funded through: the ELECTRA project [grant agreement no. 826244], which was financially supported by the Horizon 2020 programme of the European Union; the NSFC-EU Environmental Biotechnology joint program (No. 31861133001); the Key Research and Development Project of Shandong Province (No. 2020CXGC011202). S.P is a Serra Húnter Fellow (UdG-AG-575) and acknowledges the funding from the ICREA Academia award. LEQUiA [2017-SGR-1552] has been recognized as consolidated research group by the Catalan Government Open Access funding provided thanks to the CRUE-CSIC agreement with Elsevier

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.

Constructed wetlands (CWs) integrated with sulfur autotrophic denitrification to stimulate high-rate nitrogen removal from carbon-limited wastewater holds particular application prospect due to no excessive carbon source addition, high efficiency, and good stability. In this study, we conducted elemental sulfur-based constructed wetland (SCW) and traditional constructed wetland (CW) under different C/N (2, 1, and 0.5) to explore the feasibility and mechanisms for nitrogen removal from low C/N wastewater. Compared with CW, SCW was demonstrated more robust in nitrogen removal in the case of low C/N influent. When the influent C/N control was at 0.5, SCW observed total nitrogen (TN) and nitrate removal efficiency of 69.36 ± 3.96% and 81.71 ± 3.96%, with the corresponding removal rate of 1.18 ± 0.66 and 1.70 ± 0.92 g-N·m

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/m

The pathways and intermediates of continuous sulfur biotransformation in an anaerobic and anoxic sequential batch reactor (AA-SBR) involving sulfate reduction (SR) and denitrifying sulfide oxidization (DSO) were investigated. In the anoxic phase, DSO occurred in two sequential steps, the oxidation of sulfide (S2-) to elemental sulfur (S0) and the oxidation of S0 to sulfate (SO42-). The oxidation rate of S2- to S0 was 3.31 times faster than that of S0 to SO42-, resulting in the accumulation of S0 as a desired intermediate under S2--S/NO3--N ratio (molar ratio) of 0.9:1. Although, approximately 60% of generated S0 suspended in the effluent, about 40% of S0 retained in the sludge, which could be further oxidized or reduced in anoxic or anaerobic phase. In anoxic, S0 was subsequently oxidized to SO42- under S2--S/NO3--N ratio of 0.5:1. In anaerobic, S0 coexist with SO42- (in fresh wastewater) were simultaneously reduced to S2-, and the reduction rate of SO42- to S2- was 3.17 times faster than that of S0 to S2-, resulting in a higher production of S0 in subsequent anoxic phase. Microbial community analysis indicated that SO42-/S0-reducing bacteria (e.g. Desulfomicrobium and Desulfuromonas) and S2-/S0-oxidizing bacteria (e.g. Paracoccus and Thermothrix) co-participated in continuous sulfur biotransformation in the AA-SBR. A conceptual model was established to describe these main processes and key intermediates. The research offers a new insight into the reaction processes optimization for S0 recovery and simultaneous removal of SO42- and NO3- in an AA-SBR.

This study was undertaken to design a stable easy-recoverable Fe3O4@EDTA-Ag hybrid with rich catalytic sites via wet-chemical method for the catalytic reduction of multiple dyes in wastewater. The ...

Graphene oxide(GO) membrane has the potential to become the next generation of water purification membrane, which could help to ease water crisis in many counties. However, organic membrane fouling is still difficult to avoid. In this study, we used a trace of ·OH to mitigate fouling by tuning surface functional groups of GO membrane and altering fouling layer. X-ray photoelectron spectroscopy (XPS) analysis indicated that ·OH changed the epoxide-dominated GO surface to a hydroxyl-dominated surface. The adhesion force between the GO membrane and organic microspheres decreased from 0.37 ± 0.16 mN/m to 0.08 ± 0.14 mN/m after functionalization by ·OH. Quantum mechanical simulations showed that the interaction energy of the hydroxyl-dominated GO surface with a modified alginic acid monomer was 4.07 eV, which was lower than that (5.68 eV) between the epoxide-dominated GO surface and the modified alginic acid monomer. A thicker water molecule layer formed on the hydroxyl-dominated GO surface than on the epoxide-dominated GO surface through hydrogen bonding, thus repelling organic foulants. Combined with the oxidative effect of ·OH, the current method achieved the nearly complete prevention of membrane fouling. This result could provide us a new perspective for the fouling-free membrane-based water purification process.

Nitrate is one of the most common pollutants in the water environment. A key factor for the effective control and removal of nitrate is the ability to accurately determine the nitrate concentration in groundwater and the secondary effluent of wastewater treatment plants. Here, a bioelectrochemical method for real-time detection of the nitrate was developed. In this work, a kinetic model was developed to describe the correlation between the nitrate concentration and the current. Standard addition experiments showed the relative error between indicator predictions and ion chromatographic values ranged from 3.14% to 9.74%. The monitoring results of secondary effluent showed that the system could give a good response at different nitrate concentrations. The average error of not >10.85% between the indicator predictions and ion chromatographic values was demonstrated. This study offers a new method for the development of sustainable bioelectrochemical system (BES)-based technology for the real-time detection of nitrate in groundwater and the secondary effluent.

Bioelectrochemical system with biocatalyzed cathode is regarded as a promising approach for the enhanced bio-dechlorination of chlorinated aliphatic hydrocarbons (CAHs). However, the microbial community structure variation law and the corresponding function in the cathodic biofilm in response to the different cathode potentials remain poorly understood. In this study, biocathode systems were established for trichloroethene dechlorination under four cathode potentials (−0.06, −0.26, −0.46 and −0.66 V vs standard hydrogen electrode). About 2.6–4.3 times higher dechlorination rates were obtained in biocathodes than opened circuit, verifying the efficient electrostimulated bio-dechlorination. The highest trichloroethene dechlorination rate (1.01 mmol/L·d) was observed at −0.26 V, while higher (−0.06 V) or lower potentials (−0.46/−0.66 V) resulted in the 7.2–48.9% lower dechlorination rates. Under the different cathode potentials, the similar TCE dechlorination pathway was observed with cis-1,2-dichloroethene and ethene as the major and minor dechlorination products, respectively. The correlation and sharing network analysis of bacterial community illustrated that the negative potentials facilitated the enrichment of cathode-utilizing and dechlorination populations. The highest abundance of electroactive and dechlorinating bacteria (Lactococcus, Bacillus and Pseudomonas) and the highest expression of reductive dehalogenase (pceA and tceA) were observed at −0.26 V. The expression of extracellular electron transfer related gene omcX was promoted as the potential decreased. The decreased dechlorination capacity at potentials of −0.46 and −0.66 V could possibly be attributed to the lack of H2-utilizing dechlorinators and the low expressed pceA. This study offers insights into the molecular mechanism involved in the electrostimulated bio-dechlorination of CAHs by potential regulation.

Electrostimulated hydrolysis acidification (eHA) has been used as an efficient biological pre-treatment of refractory industrial wastewater. However, the effects of electrostimulation on the function and assembly of planktonic anaerobic sludge microbial communities are poorly understood. Using 16S rRNA gene and metagenomic sequencing, we investigated planktonic sludge microbial community structure, composition, function, assembly, and microbial interactions in response to electrostimulation. Compared with a conventional hydrolysis acidification (HA) reactor, the planktonic sludge microbial communities selected by electrostimulation promoted biotransformation of the azo dye Alizarin Yellow R. The taxonomic and functional structure and composition were significantly shifted upon electrostimulation with azo dyes degraders (e.g. Acinetobacter and Dechloromonas) and electroactive bacteria (e.g. Pseudomonas) being enriched. More microbial interactions between fermenters and decolorizing and electroactive bacteria, as well as fewer interactions between different fermenters evolved in the eHA microbial communities. Moreover, the decolorizing bacteria were linked to the higher abundance of genes encoding for azo- and nitro-reductases and redox mediator (e.g. ubiquinone) biosynthesis involved in the transformation of azo dye. Microbial community assembly was more driven by deterministic processes upon electrostimulation. This study offers new insights into the effects of electrostimulation on planktonic sludge microbial community function and assembly, and provides a promising strategy for the manipulation of anaerobic sludge microbiomes in HA engineering systems.

Elemental sulfur (S

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.

Pyridine contamination poses a significant threat to human and environmental health. Due to the presence of nitrogen atom in the pyridine ring, the pi bond electrons are attracted toward it and make difficult for pyridine treatment with biological and chemical methods. In this study, coupling Fenton treatment with different biological process was designed to enhance pyridine biotransformation and further mineralization. After Fenton oxidation process optimized, pretreated pyridine was evaluated under three biological (anaerobic, aerobic and microaerobic) operating conditions. Under optimum Fenton oxidation, pyridine (30–75%) and TOC (5–25%) removal efficiencies were poor. Biological process alone also showed insignificant removal efficiency, particularly anaerobic (pyridine = 8.2%; TOC = 5.3%) culturing condition. However, combining Fenton pretreatment with biological process increased pyridine (93–99%) and TOC (87–93%) removals, suggesting that hydroxyl radical generated during Fenton oxidation enhanced pyridine hydroxylation and further mineralization in the biological (aerobic > microaerobic > anaerobic) process. Intermediates were analyzed with UPLC-MS and showed presence of maleic acid, pyruvic acid, glutaric dialdehyde, succinic semialdehyde and 4-formylamino-butyric acid. High-throughput sequencing analysis also indicated that Proteobacteria (35–43%) followed by Chloroflexi (10.6–24.3%) and Acidobacteria (8.0–29%) were the dominant phyla detected in the three biological treatment conditions. Co-existence of dominant genera under aerobic/microaerobic (Nitrospira > Dokdonella > Caldilinea) and anaerobic (Nitrospira > Caldilinea > Longilinea) systems most probably play significant role in biotransformation of pyridine and its intermediate products. Overall, integrating Fenton pretreatment with different biological process is a promising technology for pyridine treatment, especially the combined system enhanced anaerobic (>10 times) microbial pyridine biotransformation activity.

Bioelectrochemical systems (BESs) have been known as a promising technology for accelerating aromatic contaminants degradation and energy recovery. However, most existing studies concentrate on aromatics metabolized through a benzoyl-CoA pathway while those metabolized through other pathways are limited. In this work, resorcinol, a typical aromatic contaminant as well as a key central intermediate (other than benzoyl-CoA) involved in aromatics anaerobic biodegradation, was studied in BESs. Unlike the general impression of the relatively poor organic-to-current performance in the aromatics driven BESs, high efficiencies for resorcinol-fed BESs were observed with a current density and coulombic efficiency of up to 0.26 ± 0.05 mA cm−2 and 74.3 ± 10.7%, respectively. The higher performance likely correlates to the readily fermentable property of resorcinol. Analysis of microbial communities in the biofilm suggests a syntrophic interaction between resorcinol-degrading bacteria (RDB) and anode-respiring bacteria (ARB) was involved in current generation. Additional tests involving the removal of accumulated acetate through fast resorcinol feeding indicates that a mechanism based on direct utilization of resorcinol for current generation may also exist. This study extends the knowledge for the fate of aromatics in BESs and indicates that aromatics entering into the resorcinol metabolic pathway can be treated efficiently with good energy recovery efficiency in BESs.

Biogenic palladium (bio-Pd) nanoparticles have been considered as promising biocatalyst for energy generation and contaminants remediation in water and sediment. Recently, an electroactive biofilm-Pd (EAB-Pd) network, which can be used directly as electrocatalyst and show enhanced electrocatalytic performance, has exhibited tremendous application potential. However, the information regarding to the controllable biosynthetic process and corresponding catalytic properties is scarce. This study demonstrated that the catalytic performance of EAB-Pd could be influenced by Pd loading on bacteria cells (Pd/cells), which was crucial to determine the final distribution characteristic of Pd nanocrystal on EAB skeleton. For instance, the high Pd/cells (over 0.18 pg cell−1) exhibited almost 6-fold and 1.5-fold enhancement over EAB-Pds with Pd/cells below 0.03 in catalytic current toward hydrogen evolution reaction and nitrobenzene reduction, respectively. In addition, the Pd/cells was found to be affected by the synthesis factors, such as the ratio of biomass to initial Pd(II) concentration (cells/PdII) and the exposure time of EAB to Pd(II) precursor solution. The Pd/cells increased significantly as the cell/PdII ratio decreased from ~5.5 × 107 to ~1.3 × 107 cells L mg−1 or the prolongation of exposure time from 3 h to 24 h. The findings developed in this work extensively expand our knowledge for the in-situ designing biogenic electrocatalyst and provide important information for the development of its catalytic property.

Dissimilatory metal-reducing bacteria (DMRB) have a variety of c-type cytochromes (OM c-cyts) intercalated in their outer membrane, and this structure serves as the physiological basis for DMRB to carry out the extracellular electron transfer processes. Using Geobacter sulfurreducens as a model DMRB, we demonstrated that visible-light illumination could alter the electronic state of OM c-cyts from the ground state to the excited state in vivo. The existence of excited-state OM c-cyts in vivo was confirmed by spectroscopy. More importantly, excited-state OM c-cyts had a more negative potential compared to their ground-state counterparts, conferring DMRB with an extra pathway to transfer electrons to semi-conductive electron acceptors. To demonstrate this, using a TiO2-coated electrode as an electron acceptor, we showed that G. sulfurreducens could directly utilise the conduction band of TiO2 as an electron acceptor under visible-light illumination (λ > 420 nm) without causing TiO2 charge separation. When G. sulfurreducens was subject to visible-light illumination, the rate of extracellular electron transfer (EET) to TiO2 accelerated by over 8-fold compared to that observed under dark conditions. Results of additional electrochemical tests provided complementary evidence to support that G. sulfurreducens utilised excited-state OM c-cyts to enhance EET to TiO2.

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.

Traditional technologies for handling nitrogen oxides (NOx) 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...

The Nernst-Monod model is used to describe bio-anode performance with respect to the effect of the electron donor and anode potential. However, electron competition is not considered in the model, limiting its application in wastewater treatment systems. In this work, nitrate was employed to describe the influence of a competitive electron acceptor on bio-anode performance. A new dynamic model of microbial anode respiration and nitrate respiration was developed for the removal of nitrogen oxides. The competitive relationship between microbial anode respiration and nitrate respiration was investigated based on electron transfer as described by the kinetics of Nernst-Monod electron transfer and nitrate reduction. The experimental results showed that nitrate had a significant influence on microbial anode respiration. The model parameters were estimated with the experimental results obtained in a continuous-flow bioelectrochemical system (BES) fed with acetate. The simulated results revealed that nitrate respiration could indirectly affect the microbial anode respiration by altering the available substrate concentration. In addition, bacterial community analysis indicated that there were two dominant functional microorganisms coexisting in the anode chamber. The first microorganism was represented by Geobacter, which has extracellular electron-transfer abilities. The second was denitrifying bacteria, which can use the carbon sources in the anodic chamber and electrons from the electrode for nitrate reduction. This is the first time that mathematical modelling of nitrate reduction has been applied to BESs.

Some refractory organic matters or soluble microbial products remained in the effluents of refractory organic wastewater after biological secondary treatment and need an advanced treatment before final disposal. Graphene oxide (GO) was known to have potential to be the next generation membrane material. The functional organics/inorganic salts separation GO membrane preparation and application in wastewater advanced treatment could reduce energy or chemicals consumption and avoid organics/inorganic salts mixed concentrate waste problems after nanofiltration or reverse osmosis. In this study, we developed a novelty GO membrane aiming at advanced purification of organic matters in the secondary effluents of refractory organic wastewater and avoiding the organics/inorganic salts mixed concentrate waste problem. The influence of preparation conditions including pore size of support membrane, the number of GO layers and the applied pressure was investigated. It was found that for organics/inorganic salts mixture separation membrane preparation, the rejection and flux would achieve balance for the support membrane at a pore size of ~0.1μm and the number of GO layers of has an optimization value (~10 layers). A higher assemble pressure (~10bar) contributed to the acquisition of a higher rejection efficiency and lower roughness membrane. This as prepared GO membrane was applied to practical secondary effluent of a chemical synthesis pharmaceuticals wastewater. A good organic matter rejection efficiency (76%) and limited salt separation (

Pyridine and its derivatives are widely consumed and detected in the environment persistently, which can cause potential adverse impacts on environment and human health. Considering the fact that pyridine could absorb UV light at 254 nm to generate excited one, which could react with reductive radicals, promoting its structural changes, we proposed that one typical efficient advanced reduction process (ARP) which combines UV irradiation with sulfite could be used to eliminate pyridine quickly. Sulfite/UV process showed a higher pyridine removal rate with a pseudo-first-order reaction rate constant of 0.1439 min−1, which was 3 times of that in UV irradiation and 1.3 times in UV/H2O2 process. This was primarily due to reductive radicals (eaq–, H• and SO3•–) produced by UV irradiation. The removal rate of pyridine was highest in slightly alkaline environment. And the presence of oxygen, as well as certain concentration of humid acid just showed slight inhibition, indicating the possibility of application in practical environment. A positive impact was observed with increasing sulfite dosage, but it was gradually inhabited when the dosage was over 5 mM. The present study may provide an alternative efficient technology for the degradation of pyridine ring-containing substances.

Nano metal catalysts produced by bacteria has received increasing attention owing to its environmental friendly synthesis route. However, the formed metal nanoparticles are associated with poorly conductive cells and challenged to be electrochemically applied. In this study, Palladium (Pd) nanoparticles were synthesized by Shewanella oneidensis MR-1. We demonstrated the limitation of palladized cells (Pd-cells) serving as electro-catalysts can be relieved by hybridizing with the conductive carbon nanotubes (Pd-cells-CNTs hybrid). Compared to the Pd-cells, the electrochemical active surface area of Pd in Pd-cells-CNTs10 (the ratio of Pd/CNTs is 1/10 w/w) were dramatically increased by 68 times to 20.44 m2·g−1. A considerable enhancement of electrocatalytic activity was further confirmed for Pd-cells-CNTs10 as indicated by a 5-fold increase of steady state current density for nitrobenzene reduction at −0.55 V vs Ag/AgCl. These results indicate that the biogenetic palladium could has been an efficient electro-catalyst but just limited due to lacking an electron transport path (e − Bridge). This finding may also be helpful to guide the way to electrochemically use other biogenetic metal nano-materials.

A hybrid anaerobic reactor with built-in bioelectrochemical system (BES) has been verified for efficiently treating mixed azo dye wastewater, yet still facing many challenges, such as uncertain reactor construction and insufficient electron donors. In this study, an up-flow hybrid anaerobic reactor with built-in BES was developed for acid orange 7 (AO7) containing wastewater treatment. Cathode and real domestic wastewater both served as electron donor for driving azo dye decolorization. The decolorization efficiency (DE) of AO7 (200 mg/L) in the hybrid reactor was 80.34 ± 2.11% with volume ratio between anaerobic sludge and cathode (VRslu:cat) of 0.5:1 and hydraulic retention time (HRT) of 6 h, which was 15.79% higher than that in BES without sludge zone. DE was improved to 86.02 ± 1.49% with VRslu:cat increased to 1:1. Further increase in the VRslu:cat to 1.5:1 and 2:1, chemical oxygen demand (COD) removal efficiency was continuously improved to 28.78 ± 1.96 and 32.19 ± 0.62%, but there was no obvious DE elevation (slightly increased to 87.62 ± 2.50 and 90.13 ± 3.10%). BES presented efficient electron utilization, the electron usage ratios (EURs) in which fluctuated between 11.02 and 13.06 mol e−/mol AO7. It was less than half of that in sludge zone of 24.73–32.06 mol e−/mol AO7. The present work optimized the volume ratio between anaerobic sludge and cathode that would be meaningful for the practical application of this hybrid system.

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.

The biological treatment of antibiotic-containing wastewater is a mainstream process, but the antibacterial activity from the persistence of antibiotics would inhibit the biological activity and function of wastewater treatment plants and lead to the risk of transmission of antibiotic resistant bacteria and genes. In this study, UV photolysis was selected as an appropriate pretreatment technology for antibiotic-containing wastewater. It could decompose many kinds of antibiotics and was not inhibited by the coexisting organics in wastewater. The antibacterial activities of five kinds of antibiotics, which were eliminated with UV irradiation, exhibited a significantly positive correlation with their parent compound concentrations. The photodecomposition of the main functional groups in antibiotics contributed to the elimination of antibacterial activity. Defluorination was the main pathway to eliminate the antibacterial activity of antibiotics containing a fluorine substituent (e.g., florfenicol and ofloxacin), while the photoinduced opening of the β-lactam ring was the most efficient route to eliminate the antibacterial activity of β-lactam antibiotics (e.g. cefalexin, amoxicillin and ampicillin). These results demonstrated that UV photolysis could be adopted as an efficient and promising pretreatment strategy for the source control of antibiotic antibacterial activity by the decomposition of antibiotic functional groups before the biological treatment unit.

The environmental spread of antibiotic resistance genes (ARGs) from the direct application of traditional biological treatment systems for antibiotics in water is a potential public health threat. UV photolysis has been proved to be an efficient pretreatment method for antibacterial activity elimination, but the fate of antibiotic resistome in subsequent bioreactors fed with pretreated florfenicol (FLO) in synthetic wastewater is still unknown. Antibacterial activity in synthetic wastewater was effectively eliminated by UV irradiation pretreatment, and the diversity and abundance of detected ARGs in both aerobic and anaerobic bioreactors were significantly lower than those without pretreatment. Meanwhile, UV irradiation pretreatment shaped the structure and composition of sludge microbial communities in the subsequent bioreactors closer to those of the FLO-free groups. The relative abundances of Pseudomonas and Escherichia-Shigella working as the potential hosts of ARGs were significantly reduced in aerobic and anaerobic bioreactors, respectively. The significantly positive correlation between floR and intI1 and the decrease of intI1 abundance in UV photolytic pretreatment groups indicated that the horizontal transfer of floR was decreased. The study provides new insights into the effect of preferential UV photolysis as a pretreatment method on the source control of antibiotic resistome in subsequent biological treatment process.

The anaerobic technology plays a fundamental role in both energy recovery and pollutant removal from wastes. However, it usually suffers from several bottlenecks, such as low reaction rates and poor system stability. To compensate for these limitations, the use of electrical stimulation to promote the anaerobic process, named as electricity-stimulated anaerobic system (ESAS), has been recently proposed. It has been demonstrated that the ESAS can improve energy recovery and pollutant removal substantially, through the regulation of metabolic pathways and electron transfer process by electrical stimulation. This paper comprehensively reviews the research progress of ESASs, covering the application of this system for energy recovery and pollutant removal, the possible enhancement mechanisms in the view of electron transfer process, response of microorganisms under electrical stimulation, as well as the strategies to manipulate such systems. Perspectives on future trends in the development of ESASs are also discussed. It is expected that the review will attract more attention to this promising technology and contribute to its further development.

Bioelectrochemical system (BES) is a rapidly developing technology covering contamination remediation, resource recovery and power generation. Electrode biofilms play a key role in BES operation. In this work, a single chamber up-flow bioelectrochemical system (UBES) was assembled with two preinoculated anodes and two raw cathodes for azo dye wastewater treatment. Microbial community structures of these electrodes after long-term operation (more than 200 days) were carried out by high-throughput Illumina 16S rRNA gene MiSeq sequencing platform. Microorganisms belonging to Enterobacter, Desulfovibrio and Enterococcus, which are capable of bidirectional extracellular electron transfer, were found to be the dominant members in all biofilms. Neither the polarity nor the position of the electrodes obviously altered the microbial community structures. This study provides a feasible strategy to build electrode active biofilms in a BES for azo dye wastewater treatment and gives great inspirations to bring this technology closer to application.

A major challenge of employing bioelectrochemical system (BES) for reductively degrading recalcitrant contaminants in industrial wastewater is lacking sufficient electron donors. In this work, domestic wastewater (DW) was demonstrated to efficiently drive BES for implementing the decolorization of azo dye, acid orange 7 (AO7). Side benefit was the simultaneous treatment of DW. Decolorization efficiency in BES fed with DW (RDW) was found to be comparable with that either fed with glucose (RGlu) or acetate (RAc). Much lower reductant usage ratio was observed in RDW. As a result, when the ratio of electron donors to azo dye decreased to 4.4 mol COD mol−1 AO7, DE of RDW kept over 90% while DEs of RAc and RGlu were significantly dropped due to the insufficient electrons donation. Besides serving as electron donor, DW was proved to also provide some conductivity and buffer capacity. Accordingly, DE of RDW was less deteriorated when fully removing the external buffer slats. This study comprehensively revealed the feasibility and superiority of DW as a cost-effective electron donor source in BES and brings this technology closer to the practice.

A continuous stirred tank reactor with built-in bioelectrochemical system (CSTR-BES) was developed for azo dye Alizarin Yellow R (AYR) containing wastewater treatment. The decolorization efficiency (DE) of the CSTR-BES was 97.04±0.06% for 7h with sludge concentration of 3000mg/L and initial AYR concentration of 100mg/L, which was superior to that of the sole CSTR mode (open circuit: 54.87±4.34%) and the sole BES mode (without sludge addition: 91.37±0.44%). The effects of sludge concentration and sodium acetate (NaAc) concentration on azo dye decolorization were investigated. The highest DE of CSTR-BES for 4h was 87.66±2.93% with sludge concentration of 12,000mg/L, NaAc concentration of 2000mg/L and initial AYR concentration of 100mg/L. The results in this study indicated that CSTR-BES could be a practical strategy for upgrading conventional anaerobic facilities against refractory wastewater treatment.

Biogenetic nanopalladium (bio-Pd) has attracted increasing attention recently due to its economical and environmental friendly synthesis route. However, traditional bacteria suspensions formed palladium (Sus-Pd) is limited to be the electrochemical catalyst owing to the poor conductivity of bacterial cells. Herein, we demonstrated Pd nanoparticles, synthesized by electroactive Geobacter biofilm, can form a three-dimensional conductive network (EAB-Pd) that is beneficial to the electrons transfer. As a result, the EAB-Pd delivered an over 5-fold increase of current compared to the Sus-Pd in hydrogen evolution and the reductive degradation of nitro-, azo- and chloroaromatics. Superior performance of EAB-Pd was also observed in comparison with the commercial Pd catalyst. A good stability of EAB-Pd has been further confirmed under electrochemical and mechanical stresses as well as through the reuse after over 3 months of storage. This novel proposed method enables the direct electrochemical application of bio...

The development of catalysts has seen tremendous growth recently but most strategies only report utilization of catalysts for a few initial cycles without taking into account the influence of oxygen poisoning. Here, the magnetic Fe3O4@EDTA-Fe (MEFe, having a core Fe3O4 particle with EDTA-Fe coating) was investigated as a model catalyst for long-term recycling for the removal of nitrogen oxide (NOx) from NO/O2 mixture, followed by N2O recovery. The concentration of oxygen in the flue gas was found to have a strong impact on NOx absorption and catalytic response. To circumvent the oxygen poisoning, the MEFe was subjected to electrochemical treatment in the presence of neutral red (N.R.) and NO removal efficiency was ∼95 % noted. Furthermore, the surface of the catalyst degraded significantly (p

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.

Wastewater treatment plants (WWTPs) play an important role within the urban water cycle in preventing the natural water environment and human health from being negatively affected by human activities. However, wastewater treatment processes such as the discharge of effluent and indirect emissions resulting from energy or chemical production, also negatively affect the environment. Footprints have been used to track human influence on the environment through different areas of concern and have been applied in assessing the sustainability of WWTPs. A comprehensive review of footprint assessment for evaluating the wastewater treatment process in WWTPs was investigated in this article. The review showed that the carbon footprint and the water footprint were the two of the most popular footprints for evaluating the sustainability of WWTPs, and other footprint (such as nitrogen and phosphorus footprints) assessment applications were also introduced to assess the eutrophication of water bodies. To promote the application of footprint assessment on WWTP, this article regulated the study goals, frameworks, system boundary, data treatment methods, resultant interpretation process. The pros and cons of footprint assessments were discussed and investigated in detail, several suggestions were come up with for the improvement of footprint assessments. The analyzation of footprint assessments under different WWTPs revealed that wastewater treatment technologies and scales significantly impacted the footprints. Moreover, the research hotspots identified by way of a keyword network diagram showed that researchers tended to propose new indicators and models for the grey water footprint and the carbon footprint respectively, and water-carbon-energy nexus was a promising direction for future studies. Finally, two possible application scenarios, element tracing through modified footprints and management improvement through mathematical optimization, were proposed to optimize the operation strategies of WWTPs. Overall, footprint assessment research for WWTPs is still at the initial stage and needs further exploration and improvement, e.g. introducing new tools, exploring system variation under various scenarios, combining other footprints, and implementing the nexus assessment.

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.

Bioelectrochemical systems (BESs) exhibit great potential for simultaneous wastewater treatment and energy recovery. However, the efficiency of microbial electrocatalysis is fundamentally limited by the high resistance and poor biocompatibility of electrode materials. Herein, we construct a novel “binder-free” 3D biocompatible bioelectrode consists of 1D aminated carbon nanotubes (CNTs-NH2) and 2D conductive reduced graphene oxide (rGO) nanosheets through one-step electrodeposition. As expected, the maximum current density reached to 3.25 ± 0.03 mA cm−2 with the rGO@CNTs-NH2 electrode, which is 4.33-fold higher than that of a bare rGO (0.75 ± 0.01 mA cm−2), and is among the best performance reported for three-dimensional electrodes. The high microbial electrocatalytic activity is mainly attributed to the excellent performance of electron transfer and bacterial colonization, which originates from the 3D interconnecting scaffold, fast 1D CNTs “e-bridge” and positively charged surface.