As(V)在金红石TiO_2颗粒表面吸附特性及机理

通过静态动力学和热力学吸附实验,研究了温度、共存离子以及溶质的初始浓度对As(V)在金红石TiO2颗粒表面吸附的影响,探讨了As(V)在金红石TiO2颗粒表面吸附特性及机理。结果表明,在As(V)初始浓度为10 mg/L,pH为7的条件下,25℃时的吸附量0.41 mg/g高于30℃时的吸附量0.31 mg/g,As(V)在金红石TiO2上的吸附为放热过程。CaCl2和MgCl2的添加对As(V)在金红石TiO2表面吸附起到明显的促进作用。T=25℃,Ca2+或Mg2+浓度为10 mmol/L时,As(V)吸附量分别为0.64和0.56 mg/g,Ca2+比Mg2+对As(V)吸附促进作用强。As(V)在金红石TiO2的吸附等温线符合Frendlich方程,Lagergren二级动力学方程能较好地描述As(V)在金红石TiO2颗粒表面吸附的动力学过程。     

海藻酸钠微胶囊负载纳米铁吸附水中的As(Ⅴ)

利用本实验所制备的海藻酸钠微胶囊负载纳米零价铁材料(M-NZVI)对水中不同浓度的As(V)进行了吸附去除研究,并比较了不同材料的吸附等温曲线。实验结果表明,2 g/L M-NZVI在pH=6.5±0.1,常温常压条件下对5 mg/L的As(V)的吸附去除率为90.35%,吸附速率较快,在30 min即可达到吸附平衡。通过M-NZVI、Ca-ALG和NZVI的热力学对比实验可知,M-NZVI表现出优越的吸附性能。溶液吸附剂添加量、初始pH值、离子浓度等因素对M-NZVI吸附水中砷离子的效率有一定影响:在其他条件不变的情况下,As(V)的去除率随着添加量的增加而逐渐增大;M-NZVI对As(V)的最佳吸附效果在pH=6~7范围之间;溶液中高浓度Na Cl能对M-NZVI的吸附性产生较强的干扰。同时,对于As(V)≤5mg/L的溶液,M-NZVI可以不做任何处理多次利用3~4次。这些结果显示,M-NZVI是一种用于原位修复重金属污染水体的潜在理想材料。     

载钛活性炭电吸附去除Cr(Ⅵ)的研究

采用sol-gel法制备了载钛活性炭,并用于电吸附处理含铬废水.当Cr(Ⅵ)初始浓度为20 mg/L时,载钛活性炭上施加1.2 V的正向电压,电吸附3 h后的处理水水质满足国家排放标准.研究了载钛活性炭电吸附去除Cr(Ⅵ)的影响因素及TiAC的电脱附再生.     

无定型纳米TiO2吸附去除饮用水中的低浓度As(Ⅲ)

研究了纳米无定型TiO2颗粒对饮用水中低浓度的三价砷As(Ⅲ)吸附行为。纳米TiO2颗粒吸附剂的BET表面积为205 m2/g,计算的BJH吸附平均孔径为4.02 nm(4 V/A)。对起始As(Ⅲ)浓度为150μg/L的模拟含砷水,经过5h的吸附处理后残余浓度不足4μg/L,As(Ⅲ)去除率达到97%。反应起始阶段吸附速率较快,84%的As(Ⅲ)能够在20min内去除。As(Ⅲ)吸附动力学较好地符合拟二级动力学模式。最佳As(Ⅲ)吸附pH为9.3,低于此值,随酸性增加吸附速率有所降低;而高于此值的强碱性pH对吸附有强烈抑制作用。在平衡浓度较低的情形下(10～220μg/L),Lang-muir,Freundlich和Dubinin-Radushkevich(D-R)吸附等温式均可较好拟合吸附行为,但中性和弱碱性条件下更符合Fre-undlich吸附等温式;平衡浓度大于220μg/L,吸附容量随平衡浓度增加而迅速增加,最大吸附容量在低浓度下达到4.79 mg/g。     

改进水热法合成纳米Co_xFe_(3-x)O_4(0≤x≤2)及其对刚果红染料的吸附性能

采用快速水热法制备了纯相Co_xFe_(3-x)O_4(0≤x≤2)纳米颗粒,并对样品进行了XRD、EDX、FTIR、SEM、N_2吸附-脱附以及VSM表征,研究了Co含量、初始浓度和pH值对水中刚果红吸附性能的影响。实验结果表明,Co_(1.6)Fe_(1.4)O_4纳米颗粒具有最大的比表面积170.1 m2·g-1和最好的吸附性能,在pH=3,初始浓度为200 mg·L~(-1)时,饱和吸附容量达到475mg·g-1。对Co_xFe_(3-x)O_4进行了吸附过程动力学和热力学分析,该吸附过程符合准二级动力学模型,根据Langmuir等温吸附模型计算得出最大吸附容量为370.4 mg·g-1。良好的磁性能使Co_(1.6)Fe_(1.4)O_4纳米颗粒很容易从水中分离再利用,实验表明,经过多次脱附/吸附过程,Co1.6Fe1.4O4纳米颗粒对刚果红仍具有良好的吸附性能。     

pH对δ-MnO_2和水铁矿吸附As(Ⅴ)的影响

研究了初始pH对δ-MnO_2和水铁矿吸附As(Ⅴ)的动力学和热力学过程的影响。结果表明,不同初始pH对水铁矿去除As(Ⅴ)的效果影响不明显,而对δ-MnO_2去除As(Ⅴ)的效果影响较大。在相同的吸附时间下,初始pH=5.0时,As(Ⅴ)去除率最高,且随初始pH增大而降低。当初始pH=5.0时,δ-MnO_2和水铁矿对As(Ⅴ)的平衡吸附量总体上都大于初始pH=7.0或初始pH=9.0时。准二级动力学方程可以很好地描述δ-MnO_2和水铁矿吸附As(Ⅴ)的动力学过程。Freundlich方程拟合水铁矿和δ-MnO_2吸附As(Ⅴ)的过程优于Langmuir方程。     

废弃荧光灯中汞的处理

在30%的丙酮-水溶液中破碎废弃荧光灯,利用超声聚能效应辅助脱附汞,在有效捕获汞蒸气的同时脱附灯管表面大部分吸附汞。考察了丙酮水溶液浓度(C)、固液比(S/L)、超声时间(t)等因素对废弃荧光灯中汞去除效果的影响。在最佳工艺条件C=30%、S/L=240 g/L、t=30 min下,平均每根荧光灯中汞的去除量达5.028 mg。采用硫化沉淀-混凝-活性炭吸附联合工艺对含汞丙酮-水溶液进行无害化处理,实验结果表明,汞初始浓度为13.79 mg/L的废水,调节pH为2,依次投加硫化钠14.5 mg/L、聚合氯化铝290.9 mg/L、活性炭量90.9 mg/L,出水汞浓度降至26.82μg/L,去除率达99.8%,达到国家排放标准。     

鼠李糖脂对底泥三氯生脱附的影响因素

采用吸附/脱附平衡实验考察了温度对鼠李糖脂作用下三氯生(TCS)在底泥/水中分配的影响,以及鼠李糖脂浓度、泥水比、反应时间、TCS初始浓度对鼠李糖脂脱附底泥中TCS的影响;并通过Box-Behnken响应曲面法(RSM)确定了鼠李糖脂强化脱附底泥中TCS的影响因素排序、最佳脱附条件和调控策略。结果表明,在283~323 K的温度范围内,温度越高,TCS越容易向水相迁移;鼠李糖脂浓度越大、泥水比越低、时间越长、TCS初始浓度越低,越有利于鼠李糖脂脱附TCS。各影响因素作用排序为:泥水比鼠李糖脂浓度pH时间;最佳脱附条件:鼠李糖脂浓度2 996.96 mg·L~(-1)、泥水比10 g·L~(-1)、反应时间30 h及pH 7.9。此时,鼠李糖脂对底泥中TCS的最大脱附率可达90.70%。可为鼠李糖脂生物表面活性剂强化受TCS污染水体的原位修复的可行性提供判据。     

As（V）在金红石TiO2颗粒表面吸附特性及机理

通过静态动力学和热力学吸附实验，研究了温度、共存离子以及溶质的初始浓度对As（V）在金红石TiO2颗粒表面吸附的影响，探讨了As（V）在金红石TiO2颗粒表面吸附特性及机理。结果表明，在As（V）初始浓度为10mg／L，pH为7的条件下，25℃时的吸附量0．41mg／g高于30℃时的吸附量0．31mg／g，As（V）在金红石TiO，上的吸附为放热过程。CaCl2和MgCl2的添加对As（V）在金红石TiO2表面吸附起到明显的促进作用。T=25℃，Ca2＋或Mg2＋浓度为10mmol／L时，As（V）吸附量分别为0．64和0．56mg／g，Ca2＋比Mg2＋对As（V）吸附促进作用强。As（V）在金红石TiO2的吸附等温线符合Frendlich方程，Lagergren二级动力学方程能较好地描述As（V）在金红石TiO2颗粒表面吸附的动力学过程。     

新生态二氧化锰对水中三价砷去除作用的研究

研究了新生态MnO2对水中As(Ⅲ)的去除效果。结果表明:新生态MnO2对As(Ⅲ)去除率高,作用速度快,作用过程符合二级动力学方程;pH=6.5时吸附等温线符合Langmuir和Frundlich方程;pH<7时,As(Ⅲ)的去除率均达80%以上,受pH和初始浓度影响较小,且与H3AsO3的pKa无关的非特性吸附;阴离子与As(Ⅲ)有吸附竞争作用,阳离子的加入可使As(Ⅲ)的去除率接近100%。     

Preparation of various thiol-functionalized carbon-based materials for enhanced removal of mercury from aqueous solution

In this work, biochar (BC), activated carbon (AC), and graphene oxide (GO) were thiol-functionalized using 3-mercaptopropyltrimethoxysilane (3-MPTS) (named as BCS, ACS, and GOS, respectively). BCS, ACS, and GOS were synthesized mainly via the interaction between hydrolyzed 3-MPTS and surface oxygen-containing functional groups (e.g., –OH, O–C=O, and C=O) and π-π interaction. The materials before and after modification were characterized and tested for mercury removal, including sorption kinetics and isotherms, the effects of adsorbent dosage, initial pH, and ionic strength. Pseudo-second-order sorption kinetic model (R² = 0.992~1.000) and Langmuir sorption isotherm model (R² = 0.964~0.998) fitted well with the sorption data of mercury. GOS had the most –SH groups with the largest adsorption capacity for Hg²⁺ and CH₃Hg⁺ (449.6 and 127.5 mg/g), followed by ACS (235.7 and 86.7 mg/g) and BCS (175.6 and 30.3 mg/g), which were much larger than GO (96.7 and 4.9 mg/g), AC (81.1 and 24.6 mg/g), and BC (95.6 and 9.4 mg/g). GOS and ACS showed stable mercury adsorption properties at a wide pH range (2~9) and ionic strength (0.01~0.1 mol/L). Mercury maybe removed by ligand exchange, surface complexation, and electrostatic attraction.

     

Sorption and transport of trichloroethylene in caliche soil

Sorption of TCE to the caliche soil exhibited linear isotherm at the high TCE concentrations (Co = 122-1300 mg L⁻¹) but Freundlich isotherm at the low concentration range (1-122 mg L⁻¹). Sorption strength of the carbonate fraction of the soil was about 100-fold lower than the sorption strength of soil organic matter (SOM) in the caliche soil, indicating weak affinity of TCE for the carbonate fraction of the soil. Desorption of TCE from the caliche soil was initially rapid (7.6 × 10⁻⁴ s⁻¹), then continued at a 100-fold slower rate (7.7 × 10⁻⁶ s⁻¹). Predominant calcium carbonate fraction of the soil (96%) was responsible for the fast desorption of TCE while the SOM fraction (0.97%) controlled the rate-limited desorption of TCE. Transport of TCE in the caliche soil was moderately retarded with respect to the water (R = 1.75-2.95). Flow interruption tests in the column experiments indicated that the rate-limited desorption of TCE controlled the non-ideal transport of TCE in the soil. Modeling studies showed that both linear and non-linear nonequilibrium transport models provided reasonably good match to the TCE breakthrough curves (r² = 0.95-0.98). Non-linear sorption had a negligible impact on both the breakthrough curve shape and the values of sorption kinetics parameters at the high TCE concentration (Co = 1300 mg L⁻¹). However, rate-limited sorption/desorption processes dominated at this concentration. For the low TCE concentration case (110 mg L⁻¹), in addition to the rate-limited sorption/desorption, contribution of the non-linear sorption to the values of sorption kinetics became fairly noticeable.     

活性炭-微波辐照处理丁腈胶乳生产废水的研究

以活性炭-微波辐照工艺处理丁腈胶乳生产废水,考察了催化剂的种类及用量、废水初始浓度、废水初始pH值、微波辐照时间和微波功率等对废水COD去除率的影响.结果表明,采用3 g粉末活性炭处理100 mL COD浓度为3500 mg/L左右的丁腈胶乳废水,在微波辐照功率为200 W,辐照时间4 min的条件下,废水COD去除率最高可达96.6%.动力学研究表明,在最佳操作条件下的反应表观过程近似符合一级反应规律,动力学方程为In(C0/C)=0.6034t 0.9247(R=0.9926),反应速率常数k=0.6034 min-1,半衰期t1/2=1.15 min.     

Effect of deposit age on adsorption and desorption behaviors of ammonia nitrogen on municipal solid waste

Ammonia nitrogen pollution control is an urgent issue of landfill. This research aims to select an optimal refuse for ammonia nitrogen removal in landfill from the point of view of adsorption and desorption behavior. MSW (municipal solid waste) samples which deposit ages were in the range of 5 to 15 years (named as R₁₅, R₁₁, R₇, and R₅) were collected from real landfill site. The ammonia nitrogen adsorption behaviors of MSW including equilibrium time, adsorption isotherms, and desorption behaviors including equilibrium time were determined. Furthermore, the effects of pH, OM, Cu(II), Zn(II), and Pb(II) on adsorption and desorption behavior of ammonia nitrogen were conducted by orthogonal experiment. The equilibrium time of ammonia nitrogen adsorption by each tested MSW was very short, i.e., 20 min, whereas desorption process needed 24 h and the ammonia nitrogen released from refuses was much lesser than that adsorbed, i.e., accounted for 3.20 % (R₁₅), 14.32 % (R₁₁), 20.59 % (R₇), and 20.50 % (R₅) of each adsorption quantity, respectively. The maximum adsorption capacity estimated from Langmuir isotherm appeared in R₁₅-KCl, i.e., 25,000 mg kg^?1. The best condition for ammonia nitrogen removal from leachate was pH >7.5, OM 23.58 %, Cu(II) <5 mg L^?1, Zn(II) <10 mg L^?1, and Pb(II) <1 mg L^?1. Ammonia nitrogen in landfill leachate could be quickly and largely absorbed by MSW but slowly and infrequently released. The refuse deposited for 15 years could be a suitable material for ammonia nitrogen removal.     

2,4-D Mineralization in soil profiles of a cultivated hummocky landscape in Manitoba,Canada

The objective of this study was to quantify 2,4-D (2,4-dichlorophenoxyacetic acid) mineralization in soil profiles characteristic of hummocky, calcareous-soil landscapes in western Canada. Twenty-five soil cores (8 cm inner diameter, 50 to 125 cm length) were collected along a 360 m transect running west to east in an agricultural field and then segmented by soil-landscape position (upper slopes, mid slopes, lower slopes and depressions) and soil horizon (A, B, and C horizons). In the A horizon, 2,4-D mineralization commenced instantaneously and the mineralization rate followed first-order kinetics. In both the B and C horizons, 2,4-D mineralization only commenced after a lag period of typically 5 to 7 days and the mineralization rate was biphasic. In the A horizon, 2,4-D mineralization parameters including the first-order mineralization rate constant (k ₁), the growth-linked mineralization rate constant (k ₂) and total 2,4-D mineralization at the end of the experiment at 56 days, were most strongly correlated to parameters describing 2,4-D sorption by soil, but were also adequately correlated to soil organic carbon content, soil pH, and carbonate content. In both B and C horizons, there was no significant correlation between 2,4-D mineralization and 2,4-D sorption parameters, and the correlation between soil properties and 2,4-D mineralization parameters was very poor. The k ₁ significantly decreased in sequence of A horizon (0.113% day^?1) > B horizon (0.024% day^?1) = C horizon (0.026% day^?1) and in each soil horizon was greater than k ₂. Total 2,4-D mineralization at 56 days also significantly decreased in sequence of A horizon (42%) > B horizon (31%) = C horizon (27%). In the A horizon, slope position had little influence on k ₁ or k ₂, except that k ₁ was significantly greater in upper slopes (0.170% day^?1) than in lower slopes (0.080% day^?1). Neither k ₁ nor k ₂ was significantly influenced by slope position in the B or C horizons. Total 2,4-D mineralization at 56 days was not influenced by slope positions in any horizon. Our results suggest that, when predicting 2,4-D transport at the field scale, pesticide fate models should consider the strong differences in 2,4-D mineralization between surface and subsurface horizons. This suggests that 2,4-D mineralization is best predicted using a model that has the ability to describe a range of non-linear mineralization curves. We also conclude that the horizontal variations in 2,4-D mineralization at the field scale will be difficult to consider in predictions of 2,4-D transport at the field scale because, within each horizon, 2,4-D mineralization was highly variable across the twenty-five soil cores, and this variability was poorly correlated to soil properties or soil-landscape position.     

In-field variation in 2,4-D mineralization in relation to sorption and soil microbial communities

This study was undertaken to assess 2,4-D mineralization in an undulating cultivated field, along a sloping transect (458 m to 442 m above sea level), as a function of soil type, soil microbial communities and the sorption of 2,4-D to soil. The 2,4-D soil sorption coefficient (Kd) ranged from 1.81 to 4.28 L kg^?1, the 2,4-D first-order mineralization rate constant (k) ranged from 0.04 to 0.13 day^?1 and the total amount of 2,4-D mineralized at 130 days (M₁₃₀) ranged from 24 to 39%. Both k and M₁₃₀ were significantly negatively associated (or correlated) with soil organic carbon content (SOC) and Kd. Both k and M₁₃₀ were significantly associated with two fatty-acid methyl esters (FAME), i17:1 and a18, but not with twenty-two other individual FAME. Imperfectly drained soils (Gleyed Dark Grey Chernozems) in lower-slopes showed significantly lesser 2,4-D mineralization relative to well-drained soils (Orthic Dark Grey Chernozems) in mid- and upper-slopes. Well-drained soils had a greater potential for 2,4-D mineralization because of greater abundance and diversity of the microbial community in these soils. However, the reduced 2,4-D mineralization in imperfectly drained soils was predominantly because of their greater SOC and increased 2,4-D sorption, limiting the bioavailability of 2,4-D for degradation. The wide range of 2,4-D sorption and mineralization in this undulating cultivated field is comparable in magnitude and extent to the variability of 2,4-D sorption and mineralization observed at a regional scale in Manitoba. As such, in-field variations in SOC and the abundance and diversity of microbial communities are determining factors that require greater attention in assessing the risk of movement of 2,4-D by runoff, eroded soil and leaching.     

Sorption-Desorption of Atrazine and Diuron in Soils from Southern Brazil

The objective of this study was to investigate the behavior of sorption and desorption of the herbicides atrazine (6-chloro-N ²-ethyl-N ⁴-isopropyl-1,3,5-triazine-2,4-diamine) and diuron [3-(3,4-dichlorophenyl)-1,1-dimethyleurea] in soil samples from a typical lithosequence located in the municipality of Mamborê (PR), southern Brazil. Five concentrations of ¹⁴C-atrazine and ¹⁴C-diuron were used for both herbicides (0.48, 0.96, 1.92, 3.84, and 7.69 mg L^?1). Sorption of both herbicides correlated positively with the organic carbon and clay content of the soil samples. Sorption isotherms were well described by the Freundlich model. The slope values of the isotherm (N) ranged from 0.84 to 0.90 (atrazine) and from 0.75 to 0.79 (diuron) for the lithosequence samples. Sorption of diuron was high regardless of the soil texture or the concentration added. The desorption isotherms for atrazine and diuron showed good fit to the Freundlich equation (R ² ≥ 0,87). Atrazine slope values for the desorption isotherms were similar for the different concentrations and were much lower than those observed for the sorption isotherms. Significant hysteresis was observed in the herbicide desorption. When the two herbicides were compared, it was found that diuron (N = 0.06–0.22) presented more pronounced hysteresis than atrazine. The results showed that, quantitatively, a greater atrazine fraction applied to these soils remains available to be leached in the soil profile, as compared to diuron.     

Degradation and sorption of imidacloprid in dissimilar surface and subsurface soils

Degradation and sorption/desorption are important processes affecting the leaching of pesticides through soil. This research characterized the degradation and sorption of imidacloprid (1-[(6-chloro-3-pyridinyl)-methyl]-N-nitro-2-imidazolidinimine) in Drummer (silty clay loam) and Exeter (sandy loam) surface soils and their corresponding subsurface soils using sequential extraction methods over 400 days. By the end of the incubation, approximately 55% of imidacloprid applied at a rate of 1.0 mg kg^?1 degraded in the Exeter sandy loam surface and subsurface soils, compared to 40% of applied imidacloprid within 300 days in Drummer surface and subsurface soils. At the 0.1 mg kg^?1 application rate, dissipation was slower for all four soils. Water-extractable imidacloprid in Exeter surface soil decreased from 98% of applied at day 1 to > 70% of the imidacloprid remaining after 400 d, as compared to 55% in the Drummer surface soil at day 1 and 12% at day 400. These data suggest that imidacloprid was bioavailable to degrading soil microorganisms and sorption/desorption was not the limiting factor for biodegradation. In subsurface soils > 40% of ¹⁴C-benzoic acid was mineralized over 21 days, demonstrating an active microbial community. In contrast, cumulative ¹⁴CO₂ was less than 1.5% of applied ¹⁴C-imidacloprid in all soils over 400 d. Qualitative differences in the microbial communities appear to limit the degradation of imidacloprid in the subsurface soils.     

Aminocyclopyrachlor sorption-desorption and leaching from three Brazilian soils

This study aimed to evaluate the sorption-desorption and leaching of aminocyclopyrachlor from three Brazilian soils. The sorption-desorption of ¹⁴C-aminocyclopyrachlor was evaluated using the batch method and leaching was assessed in glass columns. The Freundlich model showed an adequate fit for the sorption-desorption of aminocyclopyrachlor. The Freundlich sorption coefficient [K_{f (sorption)}] ranged from 0.37 to 1.34 µmol ^(1–1/n) L^1/n kg^?1 and showed a significant positive correlation with the clay content of the soil, while the K_{f (desorption)} ranged from 3.62 to 5.36 µmol ^(1–1/n) L^1/n kg^?1. The K_{f (desorption)} values were higher than their respective K_{f (sorption)}, indicating that aminocyclopyrachlor sorption is reversible, and the fate of this herbicide in the environment can be affected by leaching. Aminocyclopyrachlor was detected at all depths (0?30 cm) in all the studied soils, where leaching was influenced by soil texture. The total herbicide leaching from the sandy clay and clay soils was <0.06%, whereas, ～3% leached from the loamy sand soil. The results suggest that aminocyclopyrachlor has a high potential of leaching, based on its low sorption and high desorption capacities. Therefore, this herbicide can easily contaminate underground water resources.