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1.
Environ Res ; 258: 119461, 2024 Jun 21.
Artigo em Inglês | MEDLINE | ID: mdl-38909945

RESUMO

Microaerobic sludge bed systems could align with low-energy, reasonable carbon-nitrogen (C/N) ratio, and synchronous removal objectives during wastewater treatment. However, its ability to treat municipal wastewater (MW) with varying low C/N ratio, low NH4+ concentration, along with managing sludge bulking and loss are still unclear. Against this backdrop, this study investigated the performance of an Upflow Microaerobic Sludge Bed Reactor (UMSR) treating MW characterized by varying low C/N ratios and low NH4+ concentrations. The study also thoroughly examined associated sludge bulking and loss, pollutant removal efficiencies, sludge settleability, microbial community structures, functional gene variations, and metabolic pathways. Findings revealed that the effluent NH4+-N concentration gradually decreased to 0 mg/L with a decrease in the C/N ratio, whereas the effluent COD was unaffected by the influent, maintaining a concentration below 50 mg/L. Notably, TN removal efficiency reached 90% when C/N ratio was 3. The decrease in the C/N ratio (C/N ratio was 1) increased microbial community diversity, with abundances of AOB, AnAOB, aerobic denitrifying bacteria, and anaerobic digestion bacteria reaching 8.34%, 0.96%, 5.07%, and 9.01%, respectively. Microorganisms' metabolic pathways significantly shifted, showing increased carbohydrate and cofactor/vitamin metabolism and decreased amino acid metabolism and xenobiotic biodegradation. This study not only provides a solution for the effluent of different pre-capture carbon processes but also demonstrates the UMSR's capability in managing low C/N ratio municipal wastewater and emphasizes the critical role of microbial community adjustments and functional gene variations in enhancing nitrogen removal efficiency.

2.
Water Res ; 261: 121996, 2024 Jun 24.
Artigo em Inglês | MEDLINE | ID: mdl-38943999

RESUMO

High-strength nitrogen and antibiotics-containing wastewater can be efficiently eliminated by simultaneous denitrification and methanogenesis (SDM). Heavy metals and antibiotics are two critical factors that can lead to horizontal transfer of antibiotic resistance genes (ARGs), which can be simultaneously detected in wastewater. Unfortunately, the impacts of heavy metals on SDM and antibiotic biodegradation have not been fully elucidated. Herein, the effects of SDM and multiple antibiotics biodegradation, extracellular polymeric substances (EPSs) and protein response mechanisms, and ARG fate under Zn(II) stress were comprehensively evaluated. The results indicated that a high level of Zn(II) (≥5 mg/L) stress significantly decreased the degradation rate of multiple antibiotics and suppressed denitrification and methanogenesis. In addition, Zn(II) exposure prompted the liberation of proteins from microbes into the EPSs, and the combination of EPSs with small molecules quenched the original fluorescent components and destroyed the protein structure. The dominant proteins can bind to both Zn(II) and multiple antibiotics through several types of chemical interactions, including metallic and hydrogen bonds, hydrophobic interactions, and salt bridges, relieving the toxicity of harmful substances. Moreover, metagenomic sequencing revealed that the abundance of zinc resistance genes (Zn-RGs), ARGs (mainly tetracyclines), and mobile genetic elements (MGEs) increased under Zn(II) stress. Mantel test illustrated that the ARGs mecD, tetT, and tetB(60) were most affected by MGEs. Moreover, molecular network analysis revealed that several MGEs can bridge metal resistance genes (MRGs) and ARGs, facilitating the horizontal transfer of ARGs. This study provides theoretical guidance for the environmental risk control of antibiotics-containing wastewater treated by an SDM system.

3.
Environ Res ; 258: 119393, 2024 Jun 09.
Artigo em Inglês | MEDLINE | ID: mdl-38857856

RESUMO

Constructed wetlands have been widely employed as a cost-effective and environmentally friendly alternative for treating primary and secondary sewage effluents. In this study, biochar and pyrite were utilized as electron donor substrates in intermittent-aerated vertical flow constructed wetlands to strengthen the nutrient and heavy metals removal simultaneously, and the response of nutrient reduction and microbial community to heavy metals stress was also explored. The results indicated that biochar addition exhibited a better nitrogen removal, while pyrite addition greatly promoted the phosphorus removal. Moreover, the high removal efficiencies of Cu2+, Pb2+ and Cd2+ (above 90%) except for Zn2+ were obtained in each system. However, the exposure of heavy metals decreased phosphorus removal while had little effect on nitrogen removal. The influent load and intermittent aeration implementation led to a significant shift in microbial community structures, but microbial biodiversity and abundance decreased under the exposure of heavy metals. Particularly, Thiobacillus and Ferritrophicum, associated with sulfur autotrophic denitrification and iron autotrophic denitrification, were more abundant in pyrite-based wetland systems.

4.
Sci Total Environ ; 931: 172898, 2024 Jun 25.
Artigo em Inglês | MEDLINE | ID: mdl-38697543

RESUMO

The production of short-chain fatty acids (SCFAs) is constrained by substrate availability and the increased fractional pressure of H2 emitted by acidogenic/fermentative bacteria during anaerobic fermentation of waste activated sludge (WAS). This study introduced a novel approach employing zero-valent iron (ZVI)-activated sulfite pretreatment combined with H2-consuming sulfate-reducing bacteria (SRB) mediation to improve SCFAs, especially acetate production from WAS fermentation. Experimental results showed that the combined ZVI-activated sulfite and incomplete-oxidative SRB (io-SRB) process achieved a peak SCFAs production of 868.11 mg COD/L, with acetate accounting for 80.55 %, which was 7.90- and 2.18-fold higher than that obtained from raw WAS fermentation, respectively. This could be firstly attributed to the SO4- and OH generated by ZVI-activated sulfite, which significantly promoted WAS decomposition, e.g., soluble proteins and carbohydrates increased 14.3- and 10.8-fold, respectively, over those in raw WAS. The biodegradation of dissolved organic matter was subsequently enhanced by the synergistic interaction and H2 transfer between anaerobic fermentation bacteria (AFB) and io-SRB. The positive and negative correlations among AFB, nitrate-reducing bacteria (NRB) and the io-SRB consortia were revealed by molecular ecological network (MEN) and Mantel test. Moreover, the expression of functional genes was also improved, for instance, in relation to acetate formation, the relative abundances of phosphate acetyltransferase and acetate kinase was 0.002 % and 0.005 % higher than that in the control test, respectively. These findings emphasized the importance of sulfate radicals-based oxidation pretreatment and the collaborative relationships of multifunctional microbes on the value-added chemicals and energy recovery from sludge fermentation.


Assuntos
Ácidos Graxos Voláteis , Fermentação , Esgotos , Sulfitos , Eliminação de Resíduos Líquidos , Esgotos/microbiologia , Sulfitos/metabolismo , Ácidos Graxos Voláteis/metabolismo , Eliminação de Resíduos Líquidos/métodos , Sulfatos/metabolismo , Hidrogênio/metabolismo , Bactérias/metabolismo , Ferro/metabolismo
5.
J Environ Manage ; 360: 121110, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38733846

RESUMO

Electro-fermentation (EF) has been extensively studied for recovering hydrogen and phosphorus from waste activated sludge (WAS), while was limited for the further application due to the low hydrogen yield and phosphorus recovery efficiency. This study proposed an efficient strategy for hydrogen and vivianite recovery from the simulated sludge fermentation liquid by sacrificial iron anode in EF. The optimum hydrogen productivity and the utilization efficiency of short chain fatty acids (SCFAs) reached 45.2 mmol/g COD and 77.6% at 5 d in pH 8. Phosphate removal efficiency achieved at 90.8% at 2 d and the high crystallinity and weight percentage of vivianite (84.8%) was obtained. The functional microbes, i.e., anaerobic fermentative bacteria, electrochemical active bacteria, homo-acetogens and iron-reducing bacteria were highly enriched and the inherent interaction between the microbial consortia and environmental variables was thoroughly explored. This work may provide a theoretical basis for energy/resource recovery from WAS in the further implementation.


Assuntos
Eletrodos , Fermentação , Hidrogênio , Ferro , Fosfatos , Esgotos , Hidrogênio/metabolismo , Ferro/química , Ferro/metabolismo , Fosfatos/química , Fosfatos/metabolismo , Eliminação de Resíduos Líquidos/métodos , Fósforo/química , Fósforo/metabolismo
6.
Water Res ; 258: 121772, 2024 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-38761600

RESUMO

Nitrate photolysis has become an efficient, low-cost and promising technology for emerging contaminants removal, while its performance and mechanism for waste activated sludge (WAS) treatment is still unknown. This study innovatively introduced nitrate photolysis for WAS disintegration, and investigated the effect of nitrate addition (150-375 mg N/L) for short-chain fatty acids (SCFAs) production during anaerobic fermentation (AF). The results showed that nitrate photolysis significantly promoted the SCFAs production from WAS, and peaked at 280.7 mg/g VSS with 7-d fermentation with 150 mg N/L addition (150N-UV), which increased by 8.8-35.0 % and 10.7-23.3 % compared with other photolysis groups and sole nitrate groups. Effective release of the soluble organics was observed in the nitrate photolysis groups during AF, especially soluble proteins, reaching 1505.4 mg COD/L at 9 d in 150N-UV group, promoted by 7.0∼15.7 % than nitrate/nitrate photolysis groups. The model compounds simulation experiment further demonstrated the positive effect of nitrate photolysis on organics hydrolysis and SCFAs accumulation. The result of the radical capture and quenching verified the reactive oxygen species contributed more compared with reactive nitrogen species. Functional group analysis confirmed the effective bioconversion of the macromolecular organics during the fermentation. Moreover, the nitrate photolysis enhanced the enrichment of the functional consortia, including anaerobic fermentation bacteria (AFB), e.g., Fnoticella, Romboutsia, Gracilibacter and Sedimentibacter, and nitrate reducing bacteria (NRB), e.g., Acinerobacter and Ahniella. The macrogenetic analysis further revealed that glycolysis, amino acid metabolism, acetate metabolism and nitrogen metabolism were the dominating metabolic pathways during fermentation, and the abundance of the relevant genes were enhanced in 150N-UV group.


Assuntos
Ácidos Graxos Voláteis , Fermentação , Nitratos , Fotólise , Esgotos , Anaerobiose , Ácidos Graxos Voláteis/metabolismo , Eliminação de Resíduos Líquidos , Reatores Biológicos
7.
Environ Res ; 252(Pt 2): 118905, 2024 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-38604480

RESUMO

Persulfate oxidation (PS) is widely employed as a promising alternative for waste activated sludge pretreatment due to the capability of generating free radicals. The product differences and microbiological mechanisms by which PS activation triggers WAS digestion through multiple modes need to be further investigated. This study comprehensively investigated the effects of persulfate oxidation activated through multiple modes, i.e., ferrous, zero-valent iron (ZVI), ultraviolet (UV) and heat, on the performance of sludge digestion. Results showed that PS_ZVI significantly accelerated the methane production rate to 12.02 mL/g VSS. By contrast, PS_Heat promoted the sludge acidification and gained the maximum short-chain fatty acids (SCFAs) yield (277.11 ± 7.81 mg COD/g VSS), which was 3.41-fold compared to that in PS_ZVI. Moreover, ferrous and ZVI activated PS achieved the oriented conversion of acetate, the proportions of which took 73% and 78%, respectively. MiSeq sequencing results revealed that PS_Heat and PS_UV evidently enriched anaerobic fermentation bacteria (AFB) (i.e., Macellibacteroides and Clostridium XlVa). However, PS_Ferrous and PS_ZVI facilitated the enrichment of Woesearchaeota and methanogens. Furthermore, molecular ecological network and mantel test revealed the intrinsic interactions among the multiple functional microbes and environmental variables. The homo-acetogens and sulfate-reducing bacterial had potential cooperative and symbiotic relationships with AFB, while the nitrate-reducing bacteria displayed distinguishing ecological niches. Suitable activation modes for PS pretreatments resulted in an upregulation of genes expression responsible for digestion. This study established a scientific foundation for the application of sulfate radical-based oxidation on energy or high value-added chemicals recovery from waste residues.


Assuntos
Oxirredução , Esgotos , Sulfatos , Eliminação de Resíduos Líquidos , Esgotos/microbiologia , Sulfatos/metabolismo , Sulfatos/química , Eliminação de Resíduos Líquidos/métodos , Bactérias/metabolismo , Bactérias/genética , Reatores Biológicos/microbiologia , Metano/metabolismo , Ácidos Graxos Voláteis/metabolismo
8.
Environ Sci Technol ; 58(6): 2847-2858, 2024 Feb 13.
Artigo em Inglês | MEDLINE | ID: mdl-38299532

RESUMO

Synergistic control of the risks posed by emerging antimicrobials and antibiotic resistance genes (ARGs) is crucial for ensuring ecological safety. Although electrogenic respiration can enhance the biodegradation of several antimicrobials and reduce ARGs accumulation, the association mechanisms of antimicrobial biodegradation (trimethoprim, TMP) with the fate of the antimicrobial resistome remain unclear. Here, the biotransformation pathway of TMP, microbial associations, and functional gene profiles (e.g., degradation, antimicrobial resistance, and electron transfer) were analyzed. The results showed that the microbial electrogenic respiration significantly enhanced the biodegradation of TMP, especially with a cosubstrate sodium acetate supply. Electroactive bacteria enriched in the electrode biofilm positively correlated with potential TMP degraders dominated in the planktonic communities. These cross-niche microbial associations may contribute to the accelerated catabolism of TMP and extracellular electron transfer. Importantly, the evolution and dissemination of overall ARGs and mobile genetic elements (MGEs) were significantly weakened due to the enhanced cometabolic biodegradation of TMP. This study provides a promising strategy for the synergistic control of the water ecological risks of antimicrobials and their resistome, while also highlighting new insights into the association of antimicrobial biodegradation with the evolution of the resistome in an electrically integrated biological process.


Assuntos
Microbiota , Trimetoprima , Trimetoprima/farmacologia , Antibacterianos/farmacologia , Bactérias/genética , Resistência Microbiana a Medicamentos/genética , Genes Bacterianos
9.
Phys Chem Chem Phys ; 26(8): 7166-7176, 2024 Feb 22.
Artigo em Inglês | MEDLINE | ID: mdl-38349087

RESUMO

The Volmer step in alkaline hydrogen evolution reactions (HERs), which supplies H* to the following steps by cleaving H-O-H bonds, is considered the rate-determining step of the overall reaction. The Volmer step involves water dissociation and adsorbed hydroxyl (*OH) desorption; Ru-based catalysts display a compelling water dissociation process in an alkaline HER. Unfortunately, the strong affinity of Ru for *OH blocks the active sites, resulting in unsatisfactory performance during HER processes. Hence, this study investigates a series of key descriptors (ΔG*H2O, ΔG*H-OH, ΔG*H, and ΔG*OH) of TM (Fe, Co, Ni, Ru, Rh, Pd, Os, Ir, or Pt)-Ru/Mo2Ti2C3O2 to systematically explore the effects of bimetallic site interactions on the kinetics of the Volmer step. The results indicate that bimetallic catalysts effectively reduced the strong adsorption of *OH on Ru sites; especially, the NiRu diatomic state shows the highest electron-donating ability, which promoted the smooth migration of *OH from Ru sites to Ni sites. Therefore, Ru, Ni and MXenes are suitable to serve as water adsorption and dissociation sites, *OH desorption sites, and H2 release sites, respectively. Ultimately, NiRu/Mo2Ti2C3O2 promotes Volmer kinetics and has the potential to improve alkaline HERs. This work provides theoretical support for the construction of synergistic MXene-based diatomic catalysts and their wide application in the field of alkaline HERs.

10.
Sci Total Environ ; 912: 168893, 2024 Feb 20.
Artigo em Inglês | MEDLINE | ID: mdl-38016562

RESUMO

This study explored a novel alternating current (AC) stimulation approach to enhance the nitrogen removal efficiency of an iron­carbon based anammox (FeC anammox) system. In the preliminary experiment, the TN removal efficiency of the AC stimulated system was 8.06 % higher than that of a DC simulated system in same current densities of 0.25 mA/cm2. Gene expression analysis revealed that the AC-stimulated system, where, compared with the anammox system alone, the expression of HZS, HDH, NarG, NirS, NorB and NosZ increased by 1.81, 2.50, 1.64, 0.23, 1.15 and 1.27 times, respectively. In the continuous experiment, the TN removal rate increased from 60.13 % to 84.34 % after AC stimulation, and the working time of the FeC materials increased to 20 days. An analysis of the mechanism revealed that the parallel connection between the capacitive reactance and filler resistance in AC might reduce the internal resistance of the system, thereby improving the actual current density received by local microorganisms, and achieving a better strengthening effect.

11.
Environ Monit Assess ; 195(12): 1399, 2023 Nov 02.
Artigo em Inglês | MEDLINE | ID: mdl-37914972

RESUMO

Heavy metal concentrations represent important pollution evaluation indices, and it is necessary to assess the potential environmental and health risks from heavy metals associated with coking wastes from coking plants. In this study, coking sludge (CS), tar residue (TR), coke powder (CP), and sulfur paste (SP) from three coking plants (Plant A, Plant B, and Plant C) in central, western, and southern Shanxi Province and from soils surrounding Plant A were selected as the research objects, and the distributions of Cu, Ni, Pb, Zn, Mn, Cd, and Cr were determined. The results showed that Cd in the four solid wastes far exceeded the soil background value by a factor of 16~195, and the contents of Pb in TR (three plants) and CS (Plant C) exceeded the soil background values 19.70-, 23.57-, 14.46-, and 12.56-fold, respectively. Similarly, the concentrations of Cu, Ni, Pb, Zn, and Cd in soils were higher than the background values by factors of 31.18, 8.35, 34.79, 29.48, and 3.43, respectively. In addition, the Cu, Ni, Pb, and Cr in the four solid wastes and soils mainly existed in the residual state. As depth increased, the overall Ni, Pb, Mn, and Cd concentrations in soils increased. The high ecological risks associated with the four solid wastes were mainly due to the enrichment of Cd. Workers in coking plants face certain Cr health risks. This study provides theoretical support for the coking industry with respect to the treatment, disposal, and management of solid wastes.


Assuntos
Coque , Metais Pesados , Poluentes do Solo , Humanos , Solo/química , Resíduos Sólidos , Cádmio , Chumbo , Poluentes do Solo/análise , Monitoramento Ambiental , Metais Pesados/análise , Medição de Risco , Esgotos/química , China
12.
J Environ Manage ; 346: 118967, 2023 Nov 15.
Artigo em Inglês | MEDLINE | ID: mdl-37714089

RESUMO

Boosting acetate production from waste activated sludge (WAS) fermentation is often hindered by the inefficient solubilization in the hydrolysis step and the high hydrogen pressure ( [Formula: see text] ) during the acidogenesis of C3-C5 short-chain fatty acid (SCFAs), i.e., propionate (HPr), butyrate (HBu) and valerate (HVa). Therefore, this study employed persulfate (PS) oxidation and C3-C5 incomplete-oxidative sulfate reducing bacteria (io-SRB) metabolizers to tailor SCFAs conversion from WAS fermentation. The decomposition efficiency, performance of SCFAs production was investigated. Results showed that the PS significantly promoted WAS decomposition, with a dissolution rate of 39.4%, which is 26.0% higher than the un-treated test. Furthermore, SCFAs yields were increased to 462.7 ± 42 mg COD/g VSS in PS-HBu-SRB, which was 7.4 and 2.2 times higher than that of un-treated and sole PS tests, respectively. In particular, the sum of acetate and HPr reached the peak value of 85%, indicating that HBu-SRB mediation promoted the biotransformation of HBu and macromolecular organics by reducing the [Formula: see text] restriction. Meanwhile, sulfate radical (SO4∙-)-based oxidation (SR-AOPs) was effective in the decomposition of WAS, the oxidative product, i.e., sulfate served the necessary electron acceptor for the metabolism of io-SRB. Further analysis of Mantel test revealed the cluster of the functional genus and their interaction with environmental variables. Additionally, molecular ecological network analysis explored the potential synergistic and competitive relationships between critical genera. Additionally, the potential synergistic and competitive relationships between critical genera was explored by molecular ecological network analysis. This study provides new insights into the integration of SR-AOPs with microbial mediation in accelerating SCFAs production from WAS fermentation.


Assuntos
Ácidos Graxos Voláteis , Esgotos , Fermentação , Acetatos , Sulfatos , Concentração de Íons de Hidrogênio , Anaerobiose
13.
Int J Biol Macromol ; 252: 126093, 2023 Dec 01.
Artigo em Inglês | MEDLINE | ID: mdl-37573910

RESUMO

Inspired by recent advances on functional modification of cellulosic materials, the crosslinking behaviors of epoxide with cellulose under the catalysis of different homogeneous catalysts including H2O, Brønsted acid, Brønsted base, Lewis acid and neutral salt were systematically investigated using density functional theory (DFT) methods with hybrid micro-solvation-continuum approach. The results showed that catalytic activity, reaction mechanism and regioselectivity are determined by the combined effect of catalyst type, electronic effect and steric hindrance. All the homogeneous catalysts have catalytic activity for the crosslinking reaction, which decreases in the order of NaOH > HCl > NCl3 > MCl2 > CH3COOH > NaCl (N = Fe3+, Al3+; M = Zn2+, Ca2+). Upon the catalysis of NaOH, hydroxyl group of cellulose is firstly deprotonated to form a carbanion-like intermediate which will further attack the less sterically hindered C atom of epoxide showing excellent regioselectivity. Acidic catalysts readily cause epoxide protonated, which suffers from nucleophilic attack of cellulose and forms the carbocation-like intermediate. Brønsted acid exhibits poor regioselectivity, however, Lewis acid shows an interesting balance between catalytic activity and regioselectivity for the crosslinking reaction, which may be attributed to the unique catalysis and stabilization effects of its coordinated H2O on the transition state structure.


Assuntos
Celulose , Compostos de Epóxi , Compostos de Epóxi/química , Solventes/química , Hidróxido de Sódio , Catálise , Ácidos de Lewis
14.
J Colloid Interface Sci ; 645: 956-963, 2023 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-37182327

RESUMO

Electrocatalysis has emerged as one of the most promising alternatives to conventional anthraquinone for preparing hydrogen peroxide (H2O2) with high energy consumption and pollution because of its simplicity, convenience, and environmental friendliness. However, the oxygen reduction reaction (ORR) generating H2O2viathe2e- path is acompetitive path for 4e-ORR to generate H2O. Therefore, it is crucial to identify an electrocatalyst with high selectivity and activity of 2e-ORR. Here, we established five machine learning (ML) models based on the adsorption free energy of O* (△G (O*)) of 149 single-atom catalysts (SACs) collected and the limiting potential (UL) of 31 SACs calculated using density functional theory (DFT) from the literature. We then obtained descriptors that could accurately describe SACs. Furthermore, 690 unknown SACs' 2e-ORR catalytic performance was well predicted. Four 2e-ORR materials with high selectivity and activity were screened: Zn@Pc-N3C1, Au@Pd-N4, Au@Pd-N1C3, and Au@Py-N3C1. We verified the UL of these SACs through DFT calculation, which was higher than the standard value, proving the ML model's validity. The ML-based method to predict the material properties with highly selective and active electrocatalysts provides an efficient, rapid, and low-cost method for discovering and designing more valuable SACs catalysts.

15.
Phys Chem Chem Phys ; 25(19): 13728-13740, 2023 May 17.
Artigo em Inglês | MEDLINE | ID: mdl-37158387

RESUMO

The electrochemical hydrogen evolution reaction (HER) in alkaline media provides an environmentally friendly industrial application approach to replace traditional fossil energy. The search for efficient, low-cost, and durable active electrocatalysts is central to the development of this area. Transition metal carbides (MXenes) have been emerging as a new family of two-dimensional (2D) materials that have great potential in the HER. Herein, density functional theory calculations are performed to systematically explore the structural and electronic properties and alkaline HER performances of Mo-based MXenes, as well as the influence of species and the coordination environment of single atoms on the improvement of the electrocatalytic activity of Mo2Ti2C3O2. The results show that Mo-based MXenes (Mo2CO2, Mo2TiC2O2, and Mo2Ti2C3O2) exhibit excellent H binding ability, while slow water decomposition kinetics hinders their HER performance. Replacing the O-terminal of Mo2Ti2C3O2 with a Ru single-atom (RuS-Mo2Ti2C3O2) could promote the decomposition of water owing to the stronger electron-donating ability of the atomic state Ru. In addition, Ru could also improve the binding ability of the catalyst to H by adjusting the surface electron distribution. As a result, RuS-Mo2Ti2C3O2 exhibits excellent HER performance with a water decomposition potential barrier of 0.292 eV and a H adsorption Gibbs free energy of -0.041 eV. These explorations bring new prospects for single atoms supported on Mo-based MXenes in the alkaline hydrogen evolution reaction.

16.
Sci Total Environ ; 878: 163157, 2023 Jun 20.
Artigo em Inglês | MEDLINE | ID: mdl-37003327

RESUMO

The influence of hydraulic retention time (HRT) on the granulation process, methane-producing capacity, microbial community structure, and pollutant removal efficiency of an up-flow anaerobic sludge blanket (UASB) with simulated municipal wastewater at a mesophilic temperature was investigated. The carbon recovery capacity of the anaerobic fermentation of municipal wastewater at mesophilic temperatures is one of the problems to be investigated for the realisation of carbon neutrality in municipal wastewater treatment plants. In this study, the HRT was gradually shortened (24-6 h), and the effluent chemical oxygen demand (COD), ammonia nitrogen, pH, volatile fatty acid concentration, and specific methanogenic activity (SMA) were investigated. The sludge morphology, the particle size distribution of the different HRT, and changes in the microbial community structure were determined by scanning electron microscopy, wet screening, and high-throughput sequencing. The results indicated that even if the COD concentration was only 300-550 mg/L, with a decrease in HRT, the proportion of granular sludge in the UASB still exceeded 78 %, and the COD removal efficiency reached 82.4 %. The SMA of granular sludge increased with an increase in the size of granules and was 0.289 g CH4-COD/(g VSS d) at an HRT of 6 h, but the proportion of dissolved methane in the effluent accounted for 38-45 % of the total methane production and the proportion of Methanothrix in UASB sludge was 82.44 %. In this study, dense granular sludge was obtained by gradually shortening the HRT to start the UASB, and the lower effluent COD reduced the load of subsequent treatment processes, which could be used as a low carbon/nitrogen ratio influent for activated carbon-activated sludge, activated sludge-microalgae, and partial nitrification-anaerobic ammonia oxidation processes.


Assuntos
Esgotos , Águas Residuárias , Esgotos/química , Anaerobiose , Eliminação de Resíduos Líquidos/métodos , Estudos de Viabilidade , Reatores Biológicos , Metano/química
17.
Bioresour Technol ; 380: 129074, 2023 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-37088430

RESUMO

Using wastepaper as external carbon sources is an optional way to achieve total nitrogen removal faced with low carbon to nitrogen ratio municipal sewage. Most of studies have primarily focused on using cellulose-rich wastes establishing the separate denitrification units to achieve in-situ fermentation, which can cause blockages and prolong the process chain. In response, a novel in-situ fermentation wastepaper-flora slow-release carbon source (IF-WF) was proposed using in the original denitrification unit. IF-WF could be efficiently utilized in situ and the denitrification rate increased with the increase of nitrate nitrogen. The fermentation products were highly available, but internal acidification of IF-WF inhibited fermentation. Moreover, IF-WF limited the growth of polysaccharides in the extracellular polymeric substances of denitrified sludge. IF-WF finally formed the structure dominated by nitrate-reduction bacteria outside and cellulose-degrading bacteria inside. These results provide guidance for understanding the mechanism of IF-WF for in-situ fermentation to promote nitrogen removal.


Assuntos
Reatores Biológicos , Desnitrificação , Fermentação , Eliminação de Resíduos Líquidos , Nitratos , Carbono , Esgotos/química , Compostos Orgânicos , Nitrogênio , Celulose
18.
Chemosphere ; 325: 138336, 2023 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-36921773

RESUMO

Deposition of bimetals on Z-scheme photocatalysts has been reported to improve the nitrate nitrogen (NO3-) reduction properties. However, it is not clear whether bimetal deposition possesses advantage over single metal deposition and what is the different reaction mechanisms. In this work, the g-C3N4(Pd-Cu)/rGO/TiO2 and g-C3N4(Ag)/rGO/TiO2 composites with bimetallic Pd-Cu and single metal Ag deposited on the graphitic carbon nitride/reduced graphene oxide/titanium dioxide (g-C3N4/rGO/TiO2) Z-scheme photocatalyst were prepared, and their photocatalytic NO3- reduction properties and the mechanisms under visible light irradiation were studied. The results showed that the NO3- and total nitrogen (TN) removal efficiencies of g-C3N4(Pd-Cu)/rGO/TiO2 were 57.78% and 20.1%, respectively, 1.15 and 1.72 times higher than those of g-C3N4(Ag)/rGO/TiO2. This can be ascribed to that Pd-Cu enriched more electrons and absorbed more NO3- molecules due to the different charge densities, and the NO3- reduction process were enhanced by the staged NO3-→NO2- and NO2-→N2/NH4+ processes on Cu and Pd. The effects of reductive species were demonstrated to be photogenerated electrons > ·OH (·CO2-) > ·O2- in g-C3N4(Ag)/rGO/TiO2, while it was photogenerated electrons > ·O2- > ·OH (·CO2-) in g-C3N4(Pd-Cu)/rGO/TiO2, which may be caused by the better O2 reduction property of the latter. Finally, the cyclic experiment proved the good stability of both materials. This work provided some reference for design of metal deposited Z-scheme photocatalysts for various reduction reactions.


Assuntos
Nitratos , Dióxido de Carbono , Nitrogênio , Dióxido de Nitrogênio , Compostos Orgânicos , Metais/química
19.
Chemosphere ; 320: 138085, 2023 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-36758818

RESUMO

The investigation into the degradation of alkylphenol pollutants (APs) has become a hotspot due to their harmful effects on the environment and human health. In this study, microbial electrolysis cells (MECs) were used to degrade nonylphenol (NP) and 4-tert-octylphenol (4-tert-OP). The study found that the degradation rates of NP and 4-tert-OP for a 6-day period were 83.6% and 96.3%, respectively, which were 30.53% and 26.7% higher than those of the group without applied voltage. The double layer area in the degradation of 4-tert-OP was larger than that of NP, and the resistance exhibited by 4-tert-OP (87.47 Ω) in MEC was lower than that of NP (99.42 Ω). Meanwhile, NP had a greater effect on the bioenzyme activity than 4-tert-OP. GC-MS analysis showed that the degradation pathways of both pollutants mainly included oxidation and hydroxylation reactions. Furthermore, the microbial community analysis indicated that the main functional bacteria in NP degradation were Citrobacter, Desulfovibrio and Advenella, and those in 4-tert-OP degradation were Stenotrophomonas, Chryseobacterium, Dokdonella, and the key microbiomes underlying the cooperative relationship. The biotoxicity test indicated that the toxicity of residual substances was significantly reduced. Therefore, the MEC system is efficient and environmentally friendly and has broad application prospects in phenol refractory organics.


Assuntos
Poluentes Ambientais , Fenóis , Humanos , Anaerobiose , Fenóis/análise , Poluentes Ambientais/análise
20.
Sci Total Environ ; 861: 160795, 2023 Feb 25.
Artigo em Inglês | MEDLINE | ID: mdl-36493824

RESUMO

Persulfate has been applied extensively for waste activated sludge (WAS) decomposition due to the strong oxidizing sulfate radical generated as a product. However, the efficiency is not improved without activation to produce free radicals. In this study, a novel coupling strategy of heat-activated persulfate (Heat_PS) pretreatment and sulfate-reducing bacteria (SRB) triggering was explored to enhance short-chain fatty acids (SCFAs) produced by WAS fermentation. The remaining sulfate acts as an essential acceptor of electrons for the metabolism of synergistic SRB, thereby boosting WAS acidification by energetic cooperation with anaerobic fermenters. The results showed that SCFAs yield in the Heat_PS + SRB group peaked at 431.89 mg COD/gVSS, with the proportion of acetate reaching 57.8 %. This was 6.33 and 1.75 times higher than that in raw and single Heat_PS treated WAS, respectively. Carbon balance revealed a conversion rate of 26.1 % of carbon content in WAS to SCFAs, with 4.5 % lower CO2 equivalents emitted than that in raw WAS fermentation by the assessments of environmental impacts. This was partially attributed to the strong decomposition of WAS by SO4•- and •OH oxidation from heat-activated PS and the SRB trigger. In addition, the synergistic relationship among acidogenic/fermentative bacteria and SRB consortia was further verified by the positive correlation among Desulfovibrio, the hydrolytic Escherichia-Shigella, Morganella and the fermetative Macellibacteroides and Bacteroides, as revealed by molecular ecological networks (MENs) analysis. The results of this study may highlight the cooperation of the synergistic micribial consortia as an additional perspective for the recovery of value-added biological metabolites from complex biotransformation.


Assuntos
Desulfovibrio , Esgotos , Fermentação , Esgotos/microbiologia , Consórcios Microbianos , Temperatura Alta , Ácidos Graxos Voláteis , Óxidos de Enxofre , Sulfatos , Carbono , Concentração de Íons de Hidrogênio
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