Enhanced Adsorption of Sulfonamides by Attapulgite-Doped Biochar Prepared with Calcination.

The extensive use of sulfonamides seriously threatens the safety and stability of the ecological environment. Developing green inexpensive and effective adsorbents is critically needed for the elimination of sulfonamides from wastewater. The non-modified biochar exhibited limited adsorption capacity for sulfonamides. In this study, the attapulgite-doped biochar adsorbent (ATP/BC) was produced from attapulgite and rice straw by calcination. Compared with non-modified biochar, the specific surface area of ATP/BC increased by 73.53−131.26%, and the average pore width of ATP/BC decreased 1.77−3.60 nm. The removal rates of sulfadiazine and sulfamethazine by ATP/BC were 98.63% and 98.24%, respectively, at the mass ratio of ATP to rice straw = 1:10, time = 4 h, dosage = 2 g∙L−1, pH = 5, initial concentration = 1 mg∙L−1, and temperature = 20 °C. A pseudo-second-order kinetic model (R2 = 0.99) and the Freundlich isothermal model (R2 = 0.99) well described the process of sulfonamide adsorption on ATP/BC. Thermodynamic calculations showed that the adsorption behavior of sulfonamides on the ATP/BC was an endothermic (ΔH > 0), random (ΔS > 0), spontaneous reaction (ΔG < 0) that was dominated by chemisorption (−20 kJ∙mol−1 > ΔG). The potential adsorption mechanisms include electrostatic interaction, hydrogen bonding, π−π interaction, and Lewis acid−base interactions. This study provides an optional material to treat sulfonamides in wastewater and groundwater.

Comparison of performance of two large-scale vertical-flow constructed wetlands treating wastewater treatment plant tail-water: Contaminants removal and associated microbial community.

The removal efficiency of contaminants in large-scale integrated vertical-flow constructed wetland (IVCW) and vertical-flow constructed wetland (VCW) for wastewater treatment plant (WWTP) tail-water was evaluated, and the microbial community was also investigated in this study. The results for 14 months study period indicated that 40.05% chemical oxygen demand (COD), 45.47% ammonia nitrogen (NH4+-N), 62.55% total phosphorus (TP), 55.53% total nitrogen (TN) and 57.20% total suspended solids (TSS) average removal efficiencies were achieved in the IVCW. There was a poor performance of TN removal in the VCW, with an average removal efficiency of 38.13%. There was no significant seasonal difference in TP removal, and a strong positive correlation between influent TP load and removed load. The high-throughput sequencing analysis revealed that Proteobacteria, Planctomycetes, Bacteroidetes and Acidobacteria were dominant in nature and wetland systems. The relative abundance of nitrifying bacteria, denitrifying bacteria and anammox bacteria confirmed that nitrification, denitrification and anammox may be the main processes for nitrogen removal in the IVCW.

Use of polysorbate 20 and sodium thiosulfate to enhance sewage sludge dewaterability by bioleaching.

Dewatering of sludge is a key problem that must be solved in the sewage sludge disposal industry. In this study, a series of process optimization tests were conducted to learn how to improve sludge treatment. The optimum process of sludge leaching treatment was studied in a specially designed 100-L reactor system. Four factors were investigated and nine batches of bioleaching tests were run at three levels of these factors. Orthogonal experiments showed that the effect of sludge return ratio and aeration rate on the sludge moisture content was significant and hydraulic retention time (HRT) had a clear effect, but nutrient types had a reduced effect on the moisture content of sludge. The primary and secondary order of each factor is reflux ratio > aeration rate > HRT > nutrient type. Under the optimal process, three batches of sludge were processed and the moisture content of the filter press cake was reduced to less than 60%, the organic matter content reduced to below 5%, and the concentration of heavy metals (Cu, Zn, Pb, and Cr) was much lower than the agricultural standard limit, which is suitable for landscaping, composting, and incineration power generation and other resource applications.

Evaluation of cadmium hyperaccumulation and tolerance potential of Myriophyllum aquaticum.

Enrichment of the hyperaccumulator bank is important for phytoremediation, and studying new hyperaccumulators has become a research hotspot. In this study, cadmium (Cd), the main representative factor of heavy-metal-polluted water, was the research object, and the Cd bioenrichment ability and tolerance of Myriophyllum aquaticum were studied for the first time. The experiment was conducted for 28 days by establishing experimental groups with different Cd concentrations (0, 10, 20, 40, 80, and 160 mg/L). The results show that M. aquaticum is a new Cd hyperaccumulator. There was no notable damage in the 40 mg/L Cd treatment group, and the Cd enrichment ability of M. aquaticum reached 17,970 ± 1020.01 mg/kg, while the bioconcentration factor (BCF) reached 449.25. At the same time, the antioxidant system (superoxide dismutase (SOD) and peroxidase (POD)) and proline (Pro) levels of M. aquaticum maintained normal plant physiology, but there were physiological anomalies in M. aquaticum at high concentrations and under long-term treatment. The results show that M. aquaticum has a high Cd bioenrichment ability and tolerance in water and can be used for phytoremediation of river water polluted by Cd.

Ammonium removal characteristics of heterotrophic nitrifying bacterium Pseudomonas stutzeri GEP-01 with potential for treatment of ammonium-rich wastewater.

A heterotrophic nitrifying bacterium was isolated from the activated sludge and identified as Pseudomonas stutzeri GEP-01. Strain GEP-01 exhibited an efficient heterotrophic nitrification capability and a high nitrogen utilization rate, 48 mg/L NH4+-N was removed after culturing for 24 h without NO2--N or NO3--N accumulation, and 64.7% of the NH4+-N was removed by heterotrophic nitrification. Single-factor experiments indicated that factors such as the carbon source, temperature, NH4+-N load, and inoculum size had significant effects on the ammonium removal efficiency of strain GEP-01. The preferred conditions for heterotrophic nitrification were sodium citrate, 30 °C, 40 mg/L NH4+-N, and 5% inoculum size. When the initial NH4+-N amounts were 100, 200, 500 and 1000 mg/L, the removal rates were approximately 100%, 93%, 90.4%, and 78.9%, respectively, and higher ammonium concentrations require longer culture time. Nitrogen balance demonstrated that 40% of the initial nitrogen was lost, which was probably removed in the form of gas products under optimum culture conditions, and 36.3% of NH4+-N was converted to biomass. When incubated (adding a small amount of sodium citrate as carbon source and no carbon source) in swine wastewater containing 835 mg/L of ammonium, the removal ratio reached 56.3% and 24.8%. Strain GEP-01 has potential applications in the treatment of ammonium-rich wastewater.

Comparison of nitrogen and phosphorus removal efficiency between two types of baffled vertical flow constructed wetlands planted with Oenanthe Javanica.

The environmental problems related to rural domestic sewage treatment are becoming increasingly serious, and society is also concerned about them. A baffled vertical flow constructed wetland (BVFCW) is a good choice for cleaning wastewater. Herein, a drinking-water treatment sludge-BVFCW (D-BVFCW) parallel with ceramsite-BVFCW (C-BVFCW) planted with Oenanthe javanica (O. javanica) to treat rural domestic sewage was investigated, aiming to compare nitrogen and phosphorus removal efficiency in different BVFCWs. A removal of 23.9% NH4 +-N, 24.6% total nitrogen (TN) and 76.7% total phosphorus (TP) occurred simultaneously in the D-BVFCW; 56.4% NH4 +-N, 60.8% TN and 55.2% TP respectively in the C-BVFCW. The root and plant height increased by an average of 7.9 cm and 8.3 cm, respectively, in the D-BVFCW, and by 0.7 cm and 1.1 cm, respectively, in the C-BVFCW. These results demonstrate that the D-BVFCW and C-BVFCW have different effects on the removal of N and P. The D-BVFCW mainly removed P, while C-BVFCW mainly removed N.

Preparation of sustainable non-combustion filler substrate from waterworks sludge/aluminum slag/gypsum/silica/maifan stone for phosphorus immobilization in constructed wetlands.

In this study, an artificial wetland filler matrix capable of effectively fixing phosphorus was prepared using a non-combustion process to save energy. To evaluate the adsorption performance of this filler, adsorption experiments were performed and the phosphorus adsorption mechanism characterization was studied. An alkaline environment was found to be conducive to the increase of adsorption capacity, but excessive alkalinity was not conducive to adsorption. Static adsorption experiments showed that the phosphorus removal rate could reach 95% in the simulated phosphorus-containing wastewater after adsorption completion. The adsorption process is closely simulated by the pseudo-second-kinetic adsorption model. The isothermal adsorption experiment data were consistent with the Langmuir and the Freundlich adsorption isotherms. The characterization results showed a large number of micropores and adsorption binding sites inside and on the surface of the filler. Speciation analysis on the adsorbed phosphorus revealed that chemisorption by calcium in this filler was the dominant adsorption mechanism. The research results of this study provide the basis and reference for the development of high-efficiency phosphorus removal filler in constructed wetlands.

Effect of fluoride on photosynthetic pigment content and antioxidant system of Hydrilla verticillata.

Fluoride can either inhibit or enhance the growth of aquatic macrophytes, depending upon fluoride concentration and exposure time. To investigate fluoride toxicity, the submerged plant Hydrilla verticillata was treated with various concentrations of fluoride (F) (0, 10, 20, and 40 mg/L) for different lengths of time (7, 14, 21, and 28 days). At exposure to 10 mg/L F, the content of chlorophyll, protein, and carbohydrates content increased in leaves of H. verticillata, and the activity of guaiacol peroxidase (POD) and superoxide dismutase (SOD) slightly increased in plants compared with the control. When fluoride concentration increased to 20 mg/L, the toxic effect generated by fluoride led to a reduction of chlorophyll, protein, and carbohydrates in H. verticillata, but the activity of guaiacol peroxidase and SOD and the amount of ascorbic acid (AsA) and glutathione (GSH) were enhanced significantly. After exposure to fluoride at 40 mg/L for a long period, these physiological parameters showed a sharp decrease, and inactivation was observed in H. verticillata. These results suggested that a certain concentration of fluoride induced antioxidant response, and excess fluoride induced metabolism imbalance and oxidative damage in H. verticillata.

Improvement of sewage sludge dewaterability by bioleaching in a continuous plug flow bioreactor: optimization of process parameters.

A novel process for sewage sludge bioleaching by mixed Thiobacilli (Acidithiobacillus thiooxidans and Acidithiobacillus ferrooxidans) using a 12-stage, 180 L working volume continuous plug-flow bioreactor, is presented. The objective of the present study was to assess the impact of some parameters on the sludge dewaterability and to improve the sludge dewaterability by optimization of these parameters. The parameters examined were sludge moisture content, nutrients dosage, aeration rate, and the number of reactors. The order of the influence of these factors on sludge dewaterability was found to be sludge moisture content > nutrients dosage > aeration rate > number of reactors. The optimized conditions were: sludge moisture content, 98.0%, nutrients dosage, 9 g/L, aeration rate, 8 m3/h, and 10 reactors. Confirmation experiments conducted under optimum conditions demonstrate the sludge dewaterability to be remarkably improved. After 2 days of bioleaching, the moisture of bioleached sludge cake was reduced to below 60%.

Enhancing sludge dewatering and heavy metal removal by bioleaching with Na2S2O3 as substrates.

Bioleaching has been demonstrated to be an effective technology for the removal of heavy metals and sludge dewaterability. Since bacteria gain nutrients by diffusion of soluble compounds, the insolubility of elemental sulfur may slow the growth of bacteria. Thus, it is very important to find an energy substance quickly become available to Acidithiobacillus thiooxidans. This paper studies the improvement of sludge dewaterability and heavy metal removal with sodium thiosulfate as the source of energy for Acidithiobacillus thiooxidans. Through orthogonal experiments with specific resistance to filtration (SRF) as the target index, four factors (FeSO4 dosage, Na2S2O3 dosage, sludge reflux ratio and sludge moisture content) were identified to be the important influencing parameters. The optimal conditions were: FeSO4 dosage, 8 g/L; Na2S2O3 dosage, 1.5 g/L; sludge reflux ratio, 30%; sludge moisture content, 97%. Results indicated that the SRF of the sludge decreased from 9.89 × 1012 to 1.03 × 1011 m/kg. The removal efficiencies of heavy metals Cu, Zn, Pb and Cr could reach 83%, 78%, 31% and 38% within 3 days, respectively. These results confirm the potential of sodium thiosulfate as an alternative energy substance in bioleaching to improve sludge dewaterability as well as removal of metals.

Ammonia stress on nitrogen metabolism in tolerant aquatic plant-Myriophyllum aquaticum.

Ammonia has been a major reason of macrophyte decline in the water environment, and ammonium ion toxicity should be seen as universal, even in species frequently labeled as "NH4+ specialists". To study the effects of high NH4+-N stress of ammonium ion nitrogen on tolerant submerged macrophytes and investigate the pathways of nitrogen assimilation in different organisms, Myriophyllum aquaticum was selected and treated with various concentrations of ammonium ions at different times. Increasing of ammonium concentration leads to an overall increase in incipient ammonia content in leaves and stems of plants. In middle and later stages, high concentrations of NH4+ ion nitrogen taken up by M. aquaticum decreased, whereas the content of NO3- ion nitrogen increased. Moreover, in M. aquaticum, the activities of the enzymes nitrate reductase, glutamine synthetase and asparagine synthetase changed remarkably in the process of alleviating NH4+ toxicity and deficiency. The results of the present study may support the studies on detoxification of high ammonium ion content in NH4+-tolerant submerged macrophytes and exploration of tissue-specific expression systems.

Bioleaching in batch tests for improving sludge dewaterability and metal removal using Acidithiobacillus ferrooxidans and Acidithiobacillus thiooxidans after cold acclimation.

Bioleaching is a promising technology for removal of metals from sludge and improvement of its dewaterability. Most of the previous studies of bioleaching were focused on removal of metals; bioleaching in cold environments has not been studied extensively. In this study, Acidithiobacillus ferrooxidans and Acidithiobacillus thiooxidans were acclimated at 15 °C and co-inoculated to explore the optimal conditions for improvement of sludge dewaterability and removal of metals by the sequencing batch reactors. The data show after 6 days of bioleaching at 15 °C, 89.6% of Zn, 72.8% of Cu and 39.4% of Pb were removed and the specific resistance to filtration (SRF) was reduced to ∼12%. In addition, the best conditions for bioleaching are an initial pH of 6, a 15% (v/v) inoculum concentration, and A. thiooxidans and A. ferrooxidans mixed in a ratio of 4:1. We found that bioleaching of heavy metals is closely related to final pH, while the sludge SRF is dominated by other factors. Bioleaching can be completed in 6 days, and the sludge dewaterability and removal of metals at 15 °C meet the requirements of most sewage treatment plants.

Study of bioleaching under different hydraulic retention time for enhancing the dewaterability of digestate.

Dewatering of kitchen waste digestate is a key problem to solve so as to increase the application of kitchen waste after anaerobic digestion. In this study, the effects of bioleaching under different hydraulic retention time (HRT = 2, 2.5, and 3 days) on dewaterability of kitchen waste digestate were evaluated. A 12-stage plug flow bioreactor with 180 L working volume was used for digestate bioleaching. The bioleached digestate under different HRTs were collected and dewatered by plate-and-frame filter press. The results showed that the moisture contents of digestate cakes were 67.87 % at 2 days of HRT, 58.06 % at 2.5 days of HRT, and 54.45 % at 3 days of HRT, respectively, indicating the longer the HRT, the lower the moisture content of filter cake. Balanced between the cost and practical need, 2.5 days can be used as the HRT in engineering application. Under the condition of HRT of 2.5 days, the pH, specific resistance to filtration (SRF), capillary suction time (CST), and sedimentation rate of digestate changed from the initial values of 8.08, 210.6 s, 23.4 × 10(12) m kg(-1) and 10 % to 3.21, 32.7 s, 2.44 × 10(12) m kg(-1) and 76.8 %, respectively. Based on the observations above, the authors conclude that bioleaching technology is an effective method to enhance digestate dewaterability and reduce the cost of subsequent reutilization.

Enhanced removal of contaminant using the biological film, anoxic-anaerobic-aerobic and electro-coagulation process applied to high-load sewage treatment.

In order to explore a new treatment process applying to decentralized domestic sewage treatment, and enhance removal of total nitrogen (TN), total phosphorus (TP) and chemical oxygen demand (COD), a novel system integrating anoxic-anaerobic-aerobic (reversed A2O) and electro-coagulation (EC) process was studied, and complex biological media (CMB) was used as suspended carrier for biofilm development. In this work, TN, TP and COD removal performance were investigated with consideration of three major factors, hydraulic retention time (HRT), organic loading rate (OLR) and sludge recycle ratio (SRR). Results showed that (1) The optimum HRT was between 8 and 12 h. The removal efficiencies of TN, TP and COD were about 68%, 95% and 95%, respectively. (2) With the increase of OLR, the removal efficiency of TN increased slowly. But it increased first and then declined for COD and TP removal. Their maximum were attained when OLR was 1.8 g(COD)/(L d), and they were 96% and 93%, respectively. (3) The optimum SRR was 75%. The COD, TN and TP removal efficiencies were about 95%, 72% and 98%, respectively. In this system, the maximum TN and COD removal were achieved in anoxic tank, but it was achieved in aerobic tank for TP removal. The EC bed enhanced the effluent quality, especially the efficiency in advanced P removal. From these results, it was concluded that the new process could be a reliable option for providing excellent effluent quality.

Autotrophic denitrification based on sulfur-iron minerals: advanced wastewater treatment technology with simultaneous nitrogen and phosphorus removal.

Autotrophic denitrification technology has many advantages, including no external carbon source addition, low sludge production, high operating cost efficiency, prevention of secondary sewage pollution, and stable treatment efficiency. At present, the main research on autotrophic denitrification electron donors mainly includes sulfur, iron, and hydrogen. In these autotrophic denitrification systems, pyrite has received attention due to its advantages of easy availability of raw materials, low cost, and pH stability. When pyrite is used as a substrate for autotropic denitrification, sulfide (S2-) and ferrous ion (Fe2+) in the substrate will provide electrons to convert nitrate (NO3-) in sewage first to nitrite (NO2-), then to nitrogen (N2), and finally to discharge the system. At the same time, sulfide (S2-) loses electrons to sulfate (SO42-) and ferrous ion (Fe2+) loses electrons to ferric iron (Fe3+). Phosphates (PO43-) in wastewater are chemically combined with ferric iron (Fe3+) to form ferric phosphate (FePO4) precipitate. This paper aims to provide a detailed and comprehensive overview of the dynamic changes of nitrogen (N), phosphorus (P), and other substances in the process of sulfur autotrophic denitrification using iron sulfide, and to summarize the factors that affect wastewater treatment in the system. This work will provide a relevant research direction and theoretical basis for the field of sulfur autotrophic denitrification, especially for the related experiments of the reaction conversion of various substances in the system.

Contaminant removal performances on domestic sewage using modified anoxic/anaerobic/oxic process and micro-electrolysis.

The objective of this study was to enhance removal of chemical oxygen demand (COD), total nitrogen (TN) and total phosphorus (TP) from domestic sewage in a sequencing batch reactor with added new materials. A modified anoxic/anaerobic/oxic (MAAO) process, integrating a micro-electrolysis (ME) bed in an anoxic tank, and complex biological media (CBM) in anoxic, anaerobic and oxic tanks to treat domestic sewage, and their performances were investigated. The MAAO system was operated at controlled hydraulic retention time (HRT) of 8 h and mixed liquor recirculation (MLR) at 75%. The results showed that the MAAO system could effectively remove COD, TN and TP with average rates of 93%, 80% and 94%, respectively, in March, and 94%, 76% and 91%, respectively, in August. In this system, TP was primarily removed from the anoxic tank regardless of the operational conditions; removal contribution ratios to TP of the anoxic tank reached 56% both in March and August, indicating that the ME bed can effectively enhance phosphorus removal. TN was primarily removed from the anoxic and anaerobic tanks; removal contribution ratios to TN of anoxic and anaerobic tanks reached 36-38% and 37-38%, respectively. The oxic tank had the highest share of COD removal (56% both in March and August) in the removal of phosphorus. The outflow concentrations of COD, TN and TP were 3-46, 7-14 and 0.3-0.5 mg/L, respectively, in March, and 26-49, 9-15 and 0.04-0.1 mg/L, respectively, in August. COD and TN removal performances indicated that the innovative materials of the ME bed and CBM can effectively enhance COD and TN removal.

Treatment of high-phosphorus load wastewater by column packed with non-burning compound filler/gravel/ceramsite: evaluation of performance and microorganism community.

Cost-effective and environmental-friendly substrates are essential for the constructed wetlands (CWs). In this study, the column test was used to explore the differences in pollutant purification performance, microbial community structure and abundance between non-burning compound filler and conventional CWs substrates (i.e. gravel and ceramsite) at low temperature (0-15℃). It was found that the maximum phosphorus removal efficiency of compound filler (99%) was better than gravel (18%) and ceramsite (21%). Besides, the proportion of aerobic heterotrophic bacteria capable of ammonium oxidation, nitrification and denitrification (i.e. Pseudomonas, Acinetobacter, and Acetoanaerobium) was enhanced by compound filler, which has an excellent potential for nitrogen removal in the subsequent purification process. These results demonstrated that the self-made non-burning compound filler was a potential substrate for CWs, which was of great significance for the resource utilization of solid wastes such as polyaluminum chloride residue.

Removal of fluoride from water by five submerged plants.

Studies were conducted on the bioconcentration of fluoride (F(-)) in five submerged plants species. Ceratophyllum demersum, Hydrilla verticillata, Potamogeton malaianus, Myriophyllum verticillatum and Elodea nuttallii were all able to remove F(-) from water to some degree of efficiencies. At 5-20 mg F(-)/L culture solution, C. demersum had the best F(-)-removal performance, E. nuttallii had the poorest F(-)-removal performance among these plants. The relative growth rate (RGR) of the five species varied in different concentrations of F(-), of which C. demersum had the highest RGR. Its RGR decreased by 26.3 %, 63.2 % and 73.7 % from controls at 5, 10 and 20 mg F/L, respectively.

Preparation of a novel non-burning polyaluminum chloride residue(PACR) compound filler and its phosphate removal mechanisms.

As an inevitable industrial by-product, polyaluminum chloride residue (PACR) will cause serious harm to the environment if directly buried and dumped. The aim of this paper was searched a new economical, environmental, and practical way of utilization for PACR. In this paper, a novel non-burning PACR compound filler was made from mainly PACR. The prepared compound filler has excellent physical properties and phosphate adsorption efficiency of up to 99.9%. Static adsorption experiments showed that the adsorption process of phosphorus by the compound filler conformed to the pseudo-second-order kinetic model and intra-particle diffusion model. Langmuir and Freundlich isotherm models described the phosphorus adsorption process well, and the maximum phosphate adsorption capacity arrived at 42.55 mg/g. The phosphate adsorption by the compound filler is a spontaneous endothermic process. The main mechanisms are ligand exchange and Lewis acid-base interactions; calcium and aluminum play important roles in the adsorption of phosphorus by the compound filler. Dynamic column experiments showed that as much as 90% of the phosphorus removal by compound filler, and the phosphorus concentration decreased from 1 to ~0.1mg/L. The results provide a new waste resource utilization method for PACR and show the good application potential of prepared compound filler in constructed wetlands.

Removal behavior and mechanism of amino/carboxylate-functionalized Fe@SiO2 for Cr(VI) and Cd(II) from aqueous solutions.

The novel iron-based reductive particles, functionalized with amino and carboxylic functional groups, were synthesized to remove Cr(VI) and Cd(II) ions from aqueous solutions. The morphological structure and surface functional groups of new composites were characterized with SEM, XRD, FTIR, BET, and other techniques. The influence of pH, initial concentration, adsorbent dosing, and temperature on removal efficiencies were explored by batch experiments. The adsorption capacity of Cr(VI) and Cd(II) increased by 159.95% and 76.60%, respectively, compared with Fe0, reaching 47.638 and 62.047 mg/g. EDS and XPS analysis showed most of Cr(VI) was reduced to Cr(III) and precipitated as ferrochrome oxide, and Cd(II) was mainly precipitated as hydroxide. Reduction-precipitation and complexation may predominate in the removal process of Cr(VI), which fitted well with Langmuir and Freundlich models and pseudo-second-order kinetics. While hydrolysis and complexation may prevail for Cd(II), which was suited with Langmuir model and pseudo-second-order kinetics. Having good magnetic properties, the A/C-Fe@SiO2 particles exhibited excellent reusable stability after four times regeneration experiments, promising a prospect for in-situ remediations of groundwater contaminated by Cr(VI) and Cd(II).