Kinetics of antimony biogeochemical processes under pre-definite anaerobic and aerobic conditions in a paddy soil

While the transformation of antimony(Sb) in paddy soil has been previously investigated, the biogeochemical processes of highly chemical active Sb in the soil remain poorly understood. In addition, there is a lack of quantitative understanding of Sb transformation in soil. Therefore, in this study, the kinetics of exogenous Sb in paddy soils were investigated under anaerobic and aerobic incubation conditions. The dissolved Sb(V) and the Sb(V) extracted by diffusive gradient technique decreased u...     

Induced transformation of antimony trioxide by Mn(II) oxidation and their co-transformed mechanism

Antimony (Sb) is a toxic and carcinogenic element that often enters soil in the form of antimony trioxide (Sb₂O₃) and coexists with manganese (Mn) in weakly alkaline conditions. Mn oxides such as birnessite have been found to promote the oxidative dissolution of Sb₂O₃, but few researches concerned the co-transformations of Sb₂O₃ and Mn(II) in environment. This study investigated the mutual effect of abiotic oxidation of Mn(II) and the coupled oxidative dissolution of Sb₂O₃. The influencing factors, such as Mn(II) concentrations, pH and oxygen were also discussed. Furthermore, their co-transformed mechanism was also explored based on the analysis of Mn(II) oxidation products with or without Sb₂O₃ using XRD, SEM and XPS. The results showed that the oxidative dissolution of Sb₂O₃ was enhanced under higher pH and higher Mn(II) loadings. With a lower Mn(II) concentration such as 0.01 mmol/L Mn(II) at pH 9.0, the improved dissolution of Sb₂O₃ was attributed to the generation of dissolved intermediate Mn(III) species with strong oxidation capacity. However, under higher Mn(II) concentrations, both amorphous Mn(III) oxides and intermediate Mn(III) species were responsible for promoting the oxidative dissolution of Sb₂O₃. Most released Sb (∼72%) was immobilized by Mn oxides and Sb(V) was dominant in the adsorbed and dissolved total Sb. Meanwhile, the presence of Sb₂O₃ not only inhibited the removal of Mn(II) by reducing Mn(III) to Mn(II) but also affected the final products of Mn oxides. For example, amorphous Mn oxides were formed instead of crystalline Mn(III) oxides, such as MnOOH. Furthermore, rhodochrosite (MnCO₃) was formed with the high Mn(II)/Sb₂O₃ ratio_, but without being observed in the low Mn(II)/Sb₂O₃ ratio. The results of study could help provide more understanding about the fate of Sb in the environment and the redox transformation of Mn.     

Identification of potential electrotrophic microbial community in paddy soils by enrichment of microbial electrolysis cell biocathodes

Electrotrophs are microbes that can receive electrons directly from cathode in a microbial electrolysis cell(MEC).They not only participate in organic biosynthesis,but also be crucial in cathode-based bioremediation.However,little is known about the electrotrophic community in paddy soils.Here,the putative electrotrophs were enriched by cathodes of MECs constructed from five paddy soils with various properties using bicarbonate as an electron acceptor,and identified by 16 S rRNA-gene based Illum...     

Effects of natural organic matter on cadmium mobility in paddy soil: A review

Cadmium (Cd) contamination in paddy soil has caused public concern. The uptake of Cd by rice plants depends on soil Cd mobility, which is in turn substantially influenced by organic matter (OM). In this review, we first summarize the fate of Cd in soil and the role of OM. We then focus on the effects of OM on Cd mobility in paddy soil and the factors influencing the remedial effectiveness of OM amendments. We further discuss the performance of straw incorporation in the remediation of Cd-contaminated paddy soils reported in laboratory and field studies. Considering the huge production of organic materials (such as straw) in agriculture, the use of natural OM for soil remediation has obvious appeal due to the environmental benefits and low cost. Although there have been successful application cases, the properties of OM amendments and soil can significantly affect the remedial performance of the OM amendments. Importantly, straw incorporation alone does not often decrease the mobility of Cd in soil or the Cd content in rice grains. Careful evaluation is required when considering natural OM amendments, and the factors and mechanisms that influence their remedial effectiveness need further investigation in paddy soil with realistic Cd concentrations.     

Combined effects of volume ratio and nitrate recycling ratio on nutrient removal, sludge characteristic and microbial evolution for DPR optimization

The optimization of volume ratio (V_An/V_A/V_O) and nitrate recycling ratio (R) in a two-sludge denitrifying phosphorus removal (DPR) process of Anaerobic Anoxic Oxic-Moving Bed Biofilm Reactor (A²/O-MBBR) was investigated. The results showed that prolonged anaerobic retention time (HRT_An: 1.25→3.75 hr) exerted favorable effect on chemical oxygen demand (COD) removal (57.26%→73.54%), poly-β-hydroxyalkanoates (PHA) synthesis (105.70→138.12 mgCOD/L) and PO₄^3? release (22.3→38.9 mg/L). However, anoxic retention time (HRT_A) and R exhibited positive correlation with PHA utilization (43.87%-81.34%) and denitrifying phosphorus removal (DPR) potential (ΔNO₃^?/ΔPO₄^3?: 0.57-1.34 mg/mg), leading to dramatical TN removal variations from 68.86% to 81.28%. Under the V_An/V_A/V_O ratio of 2:6:0, sludge loss deteriorated nutrient removals but the sludge bioactivity quickly recovered when the oxic zone was recovered. The sludge characteristic and microstructure gradually transformed under the dissolved oxygen (DO) control (1.0-1.5→1.5-2.0 mg/L), in terms of sludge volume index (SVI: 194→57 mL/gVSS), median-particle-size (D₅₀: 99.6→300.5 μm), extracellular polymeric substances (EPS) (105.62→226.18 mg/g VSS) and proteins/polysaccharides (PN/PS) ratio (1.52→3.46). Fluorescence in situ hybridization (FISH) results showed that phosphorus accumulation organisms (PAOs) (mainly Cluster I of Accumulibacter, contribution ratio: 91.79%-94.10%) dominated the superior DPR performance, while glycogen accumulating organisms (GAOs) (mainly Competibacter, contribution ratio: 82.61%-86.89%) was responsible for deteriorative TN and PO₄^3? removals. The optimal HRT_A and R assembled around 5-6.5 hr and 300%-400% based on the PHA utilization and DRP performance, and the oxic zones also contributed to PO₄^3? removal although it showed low dependence on DO concentration and oxic retention time (HRT_O).     

Spatiotemporal variations of nitrate sources and dynamics in a typical agricultural riverine system under monsoon climate

Nitrogen pollution is a serious environmental issue in the Danjiangkou Reservoir region(DRR),the water source of the South-to-North Water Diversion Project of China.In this research,seasonal surveys and a bi-weekly time series survey were conducted in the Qihe River Basin,one of the most densely populated agricultural basins in the DRR.Hydrochemical compositions (NO₃Cl),dual isotopes (δD-H₂O,δ¹⁸O-H₂O,δ¹⁵N-NO₃^-,and δ     

Conversion of nitrogen and carbon in enriched paddy soil by denitrification coupled with anammox in a bioelectrochemical system

The aim of this study is to investigate conversion of nitrogen and COD in enriched paddy soil by nitrification coupled with anammox process in a dual chamber bioelectrochemical system. The paddy soil was enriched for denitrification coupled with anammox by microbial consortia and was acclimatized in the cathodic chamber of microbial fuel cells(MFCs). The bioelectrochemical systems were treated with different ammonium concentrations in the cathodic chamber: the MFC with low concentration ammonium...     

土壤调理剂对土壤-水稻系统Cd、Zn迁移累积的影响及健康风险评价

选取湖南省长沙市北山镇某中重度Cd污染稻田,研究了土壤调理剂(石灰石+偏高岭土+钙镁磷肥)对稻田土壤重金属Cd、Zn的钝化效果,以及对水稻各部位累积Cd和Zn的影响,并进行了Cd的健康风险评价.结果表明,使用土壤调理剂提高了稻田土壤p H值.Cd的CaCl_2提取态含量降低了0.9%~24.1%,Zn的CaCl_2提取态含量降低了22.5%~69.6%.土壤调理剂显著降低了水稻糙米中Cd与Zn的含量,与对照相比分别降低了10.8%~47.3%、10.3%~17.5%;土壤调理剂对水稻糙米Cd的吸收和累积的影响要远大于Zn,水稻糙米中的Cd/Zn比随着土壤调理剂施用量的增加而显著降低.研究区大米重金属Cd目标危害系数THQ值大于1,说明当地人群通过食用大米途径摄入重金属Cd存在健康风险.土壤调理剂有效地抑制了水稻植株对土壤中Cd的吸收,并降低了Cd/Zn比,使糙米中的Cd含量显著降低,从而降低了当地人群通过食用大米途径摄入重金属Cd的健康风险.     

Mixing regime shapes the community assembly process, microbial interaction and proliferation of cyanobacterial species Planktothrix in a stratified lake

Lake mixing influences aquatic chemical properties and microbial community composition,and thus, we hypothesized that it would alter microbial community assembly and interaction. To clarify this issue, we explored the community assembly processes and cooccurrence networks in four seasons at two depths(epilimnion and hypolimnion) in a mesotrophic and stratified lake(Chenghai Lake), which formed stratification in the summer and turnover in the winter. During the stratification period, the epilimni...     

Effect of allelochemicals sustained-release microspheres on the ingestion,incorporation, and digestion abilities of Daphnia magna Straus

Allelochemicals sustained-release microspheres (ACs-SMs) exhibited great inhibition effect on algae,however,few studies have focused on ACs-SMs toxicity on invertebrate.In this study,the effects of single high-concentration ACs (15 mg/L,SH-ACs),repeated low-concentration ACs (3×5 mg/L,RL-ACs) and ACs-SMs containing 15 mg/L ACs exposure on the ingestion,incorporation,and digestion of Daphnia magna Straus (DS) were investigated by stable isotope¹⁵N labeling method.Meanwhile,the diversit...     

Phase transformation of Cr(VI)-adsorbed ferrihydrite in the presence of Mn(II): Fate of Mn(II) and Cr(VI)

Ferrihydrite is an important sink for the toxic heavy metal ions, such as Cr(VI). As ferrihydrite is thermodynamically unstable and gradually transforms into hematite and goethite, the stability of Cr(VI)-adsorbed ferrihydrite is environmentally significant. This study investigated the phase transformation of Cr(VI)-adsorbed ferrihydrite at different pH in the presence of aqueous Mn(II), as well as the fate of Mn(II) and Cr(VI) in the transformation process of ferrihydrite. Among the ferrihydrite transformation products, hematite was dominant, and goethite was minor. The pre-adsorbed Cr(VI) inhibited the conversion of ferrihydrite to goethite at initial pH 3.0, whereas little amount of adsorbed Mn(II) favored the formation of goethite at initial pH 7.0. After the aging process, Cr species in solid phase existed primarily as Cr(III) in the presence of Mn(II) at initial pH 7.0 and 11.0. The aqueous Mn concentration was predominantly unchanged at initial pH 3.0, whereas the aqueous Mn(II) was adsorbed onto ferrihydrite or form Mn(OH)₂ precipitates at initial pH 7.0 and 11.0, promoting the immobilization of Cr(VI). Moreover, the oxidation of Mn(II) occurred at initial pH 7.0 and 11.0, forming Mn(III/IV) (hydr)oxides.     

Long-term effects of silver nanoparticles on performance of phosphorus removal in a laboratory-scale vertical flow constructed wetland

Silver nanoparticles(AgNPs) have been widely used in many fields,which raised concerns about potential threats to biological sewage treatment systems.In this study,the phosphorus removal performance,enzymatic activity and microbial population dynamics in constructed wetlands(CWs) were evaluated under a long-term exposure to Ag NPs(0,50,and 200 μg/L) for 450 days.Results have shown that Ag NPs inhibited the phosphorus removal efficiency in a short-term exposure,whereas caused no obviously negativ...     

Simultaneous oxidation of Mn(II) and As(III) on cupric oxide (CuO) promotes As(III) removal at circumneutral pH

Oxidation of Mn(II) or As(III) by molecular oxygen is slow at pH < 9, while they can be catalytically oxidized in the presence of oxide minerals and then removed from contaminated water. However, the reaction mechanisms on simultaneous oxidation of Mn(II) and As(III) on oxide mineral surface and their accompanied removal efficiency remain unclear. This study compared Mn(II) oxidation on four common metal oxides (γ-Al₂O₃, CuO, α-Fe₂O₃ and ZnO) and investigated the simultaneous oxidation and removal of Mn(II) and As(III) through batch experiments and spectroscopic analyses. Among the tested oxides, CuO and α-Fe₂O₃ possess greater catalytic activity toward Mn(II) oxidation. Oxidation and removal kinetics of Mn(II) and As(III) on CuO indicate that O₂ is the terminal electron acceptor for Mn(II) and As(III) oxidation on CuO, and Mn(II) acts as an electron shuttle to promote As(III) oxidation and removal. The main oxidized product of Mn(II) on CuO is high-valent MnO_x species. This newly formed Mn(III) or Mn(IV) phases promote As(III) oxidation on CuO at circumneutral pH 8 and is reduced to Mn(II), which may be then released into solution. This study provides new insights into metal oxide-catalyzed oxidation of pollutants Mn(II) and As(III) and suggests that CuO should be considered as an efficient material to remediate Mn(II) and As(III) contamination.     

Effects of substrate types on the transformation of heavy metal speciation and bioavailability in an anaerobic digestion system

Chemical speciation can fundamentally affect the potential toxicity and bioavailability of heavy metals. The transformation of heavy metal speciation and change of bioavailability were investigated in an anaerobic digestion (AD) system using four different substrates (pig manure (PM), cattle manure (CAM), chicken manure (CHM) and rice straw (RS)). The results obtained indicated that the total contents of heavy metals in PM, CHM and CAM were higher than in RS and decreased in the order Zn > Cu > Ni > Pb > As > Cd in all substrates. Moreover, the speciation with the largest proportion for each heavy metal was the same both in the different substrates and the biogas residues. Among them, Zn, Ni, Cd and As were mainly in the reducible fraction (F2), while Cu was mainly in the oxidizable fraction (F3) and Pb occurred predominantly in the residual fraction (F4). Our results further indicated that the AD process had a greater effect on the speciation of heavy metals in CHM and PM, but less on CAM and RS. The rates of change in bioavailability followed the order PM > CHM > CAM > RS. Changes in organic matter, humic acid or local metal ion environment as a result of AD were inferred as likely mechanisms leading to the transformation of heavy metal speciation. These results enhanced our understanding of the behavior of heavy metals in AD and provided a new perspective for the treatment and disposal of the substrates.     

Influence of modified biochar supported sulfidation of nano-zero-valent-iron (S-nZVI/BC) on nitrate removal and greenhouse gas emission in constructed wetland

In this study, the biochar (BC) produced from sawdust, sludge, reed and walnut were used to support sulfidation of nano-zero-valent-iron (S-nZVI) to enhance nitrate (${\text{NO}}_3^{-}$-N) removal and investigate the impact on greenhouse gas emissions. Batch experiment results showed the S-nZVI/BC_{sawdust (2:1, 500)}, S-nZVI/BC_{sludge (2:1, 900)}, S-nZVI/BC_{reed (2:1, 700)}, and S-nZVI/BC _{walnut (2:1, 700)} respectively improved ${\text{NO}}_3^{-}$-N removal efficiencies by 22%, 20%, 3% and 0.1%, and the selectivity toward N₂ by 22%, 25%, 22% and 18%. S-nZVI uniformly loaded on BC provided electrons for the conversion of ${\text{NO}}_3^{-}$-N to N₂ through Fe⁰. At the same time, FeS_x layer was formed on the outer layer of ZVI in the sulfidation process to prevent iron oxidation, so as to improve the electrons utilization efficiency After adding four kinds of S-nZVI/BC into constructed wetlands (CWs), the ${\text{NO}}_3^{-}$-N removal efficiencies could reach 100% and the N₂O emission fluxes were reduced by 24.17%-36.63%. And the average removal efficiencies of TN, COD, TP were increased by 21.9%, -16.5%, 44.3%, repectively. The increasing relative abundances of denitrifying bacteria, such as Comamonas and Simplicispira, suggested that S-nZVI/BC could also improve the process of microbial denitrification. In addition, different S-nZVI/BC had different effects on denitrification functional genes (narG, nirk, nirS and nosZ genes), methanotrophs (pmoA) and methanogenesis (mcrA). This research provided an effective method to improve ${\text{NO}}_3^{-}$-N removal and reduce N₂O emission in CWs.     

Biofilm response and removal via the coupling of visible-light-driven photocatalysis and biodegradation in an environment of sulfamethoxazole and Cr(VI)

The widespread contamination of water systems with antibiotics and heavy metals has gained much attention. Intimately coupled visible -light-responsive photocatalysis and biodegradation (ICPB) provides a novel approach for removing such mixed pollutants. In ICPB, the photocatalysis products are biodegraded by a protected biofilm, leading to the mineralization of refractory organics. In the present study, the ICPB approach exhibited excellent photocatalytic activity and biodegradation, providing up to ∼1.27 times the degradation rate of sulfamethoxazole (SMX) and 1.16 times the Cr(VI) reduction rate of visible-light-induced photocatalysis . Three-dimensional fluorescence analysis demonstrated the synergistic ICPB effects of photocatalysis and biodegradation for removing SMX and reducing Cr(VI). In addition, the toxicity of the SMX intermediates and Cr(VI) in the ICPB process significantly decreased. The use of MoS₂/CoS₂ photocatalyst accelerated the separation of electrons and holes, with•O₂^– and h⁺ attacking SMX and e^– reducing Cr(VI), providing an effective means for enhancing the removal and mineralization of these mixed pollutants via the ICPB technique. The microbial community results demonstrate that bacteria that are conducive to pollutant removal are were enriched by the acclimation and ICPB operation processes, thus significantly improving the performance of the ICPB system.     

贵州某锑冶炼厂周边农田土壤锑、砷污染与人体健康风险评估

本研究以贵州省独山县某锑冶炼厂周边农田土壤为研究对象,系统采集17个土壤样品,测定了土壤中Sb、As总含量,并采用生理提取试验(PBET)和简化生物可给性提取试验(SBET)两种体外胃肠模拟实验方法分析了土壤中Sb、As的生物可给态含量,基于土壤Sb、As总量和生物可给性(PBET和SBET)评估了研究区锑、砷污染土壤...     

Distribution, risk and bioavailability of metals in sediments of Lake Yamdrok Basin on the Tibetan Plateau, China

Total contents of metals in soil and sediments on the Tibetan Plateau of China have been widely analyzed, but existing information is insufficient to effectively evaluate metal ecological risk because of a lack of metal bioavailability data. In this study, distribution, potential risk, mobility and bioavailability of metals in sediments of Lake Yamdrok Basin in Tibet of China were explored by combined use of total digestion, sequential extraction and the diffusive gradient in thin-films(DGT). Av...     

Experimental and modeling investigations on the unexpected hydrogen sulfide rebound in a sewer receiving nitrate addition: Mechanism and solution

Biogenic hydrogen sulfide is an odorous, toxic and corrosive gas released from sewage in sewers. To control sulfide generation and emission, nitrate is extensively applied in sewer systems for decades. However, the unexpected sulfide rebound after nitrate addition is being questioned in recent studies. Possible reasons for the sulfide rebounds have been studied, but the mechanism is still unclear, so the countermeasure is not yet proposed. In this study, a lab-scale sewer system was developed for investigating the unexpected sulfide rebounds via the traditional strategy of nitrate addition during 195-days of operation. It was observed that the sulfide pollution was even severe in a sewer receiving nitrate addition. The mechanism for the sulfide rebound can be differentiated into short-term and long-term effects based on the dominant contribution. The accumulation of intermediate elemental sulfur in biofilm resulted in a rapid sulfide rebound via the high-rate sulfur reduction after the depletion of nitrate in a short period. The presence of nitrate in sewer promoted the microorganism proliferation in biofilm, increased the biofilm thickness, re-shaped the microbial community and enhanced biological denitrification and sulfur production, which further weakened the effect of nitrate on sulfide control during the long-term operation. An optimized biofilm-initiated sewer process model demonstrated that neither the intermittent nitrate addition nor the continuous nitrate addition was a sustainable strategy for the sulfide control. To minimize the negative impact from sulfide rebounds, a (bi)monthly routine maintenance (e.g., hydraulic flushing with nitrate spike) to remove the proliferative microorganism in biofilm is necessary.     

Responses of nitrification performance, triclosan resistome and diversity of microbes to continuous triclosan stress in activated sludge system

Triclosan(TCS) is commonly found in wastewater treatment plants,which often affects biological treatment processes.The responses of nitrification,antibiotic resistome and microbial community under different TCS concentrations in activated sludge system were evaluated in this study.The experiment was conducted in a sequencing batch reactor(SBR)for 240 days.Quantitative PCR results demonstrated that the abundance of ammonium oxidizing bacteria could be temporarily inhibited by 1 mg/L TCS and then ...