离子强度对外源纳米银形态转化和氨氧化细菌Nitrosomonas europaea活性的影响

以氨氧化细菌—欧洲亚硝化单胞杆菌(Nitrosomonas europaea)为模式菌株,研究纳米银(silver nanoparticles,AgNPs)在不同离子强度水样中的赋存形态及对N.europaea氧化NH₄⁺-N性能的影响。在N. europaea培养液、月牙湖水、生活污水、化工废水4种水样中分别添加AgNPs及不同形态Ag化合物,测试其对N.europaea的急性毒性,得到AgNPs及不同形态银对N.europaea的毒性效应浓度EC₂₀、EC₅₀和EC₈₀。采用紫外可见吸收光谱法分析AgNPs在不同离子强度水样中的粒径变化。利用Visual MINTEQ模型预测AgNPs在4种水样中的主要化学形态分布,发现水样的离子组分及离子强度显著影响AgNPs的聚集和Ag的赋存状态。在4种水样中分别添加不同浓度(EC₂₀、EC₅₀和EC₈₀)的AgNPs,探究不同离子强度水样中的AgNPs对N.europaea活性的影响,结果表明随着水样中外源添加AgNPs浓度的增加,N.europaea氧化NH₄⁺-N的效率降低,特别在培养液和校园生活污水中,呈现较明显的剂量效应;但在月牙湖水和化工废水中,由于其含有高浓度SO₄²⁻、Cl⁻等离子组分,影响AgNPs对N.europaea的毒性效应。评价AgNPs在环境水体或污水中的生物毒性,应考虑水中离子组成和离子强度对其毒性的影响。     

黑臭水体治理Ⅰ：水体氧状态对沉积物中重金属形态及生物有效性的影响

黑臭水体治理会逐步恢复上覆水中溶解氧浓度,基于这一过程构建了室内模拟装置,模拟上覆水不同氧状态,探究由此引发的氧化还原体系变化,及6种重金属元素(Co、Ni、Cu、As、Sb和Pb)的形态和生物有效性变化.结果表明,上覆水氧化还原电位为-109.60～+136.40 mV,主要受铁锰体系控制,好氧和厌氧阶段沉积物氧化还原电位分别为-160.40～-116.40 mV和-370.10～-250.30 mV,分别由铁锰体系和硫体系控制.上覆水中溶解氧浓度上升会引起沉积物中有效态S和Fe减少,上覆水和浅层沉积物中有效态Mn减少,而有效态Fe和Mn浓度在溶解氧浓度降低后会逐步升高,说明上覆水氧状态改变能触动上覆水和沉积物中氧化还原体系变化.但上覆水氧状态改变不足以引起上覆水和沉积物中重金属总量变化(除Sb),上覆水中Co、Ni、Cu、As、Sb和Pb总量分别为0.94～1.69、2.23～3.06、0.62～1.43、0.48～0.98、0.89～5.64、0.14～0.26μg·L^-1,沉积物中分别为17.74～18.65、26.82～29.45、54.64～57.33...     

联用技术在砷形态分析中的研究进展

摘要：目前用于元素砷的形态分析技术主要是色谱与原子光谱、质谱等的联用,最常用的是HPLC与ICP—OES、ICP—MS的联用,方法准确可靠,灵敏度高,但是不能提供砷化合物的分子结构信息。因此以色谱一电喷雾质谱（ESI—MS）的联用作为定性分析的主要手段,但是ESI—MS灵敏度低,易受基体干扰,因此需要复杂的前处理技术。     

土壤中钙、镁的形态分析及提取序列的研究

本文采用改进的BCR三步连续提取法对河北某食道癌高发地土壤中钙、镁进行了形态分析及提取序列的研究。实验表明：该地区土壤中镁主要以残渣态形式存在（占总量的83.66％-88.36％）,钙则受提取序列的影响很大,在第一提取序列中,以酸溶态为主（74.11％-83.38％）;第二提取序列中,以有机物结合态为主（78.12％-97.17％）;第三、四提取序列中,以氧化物结合态为主（87.49％-103％）。提取剂的加入顺序明显影响到钙的各个形态的真实含量。     

Study on the hydrolysis/precipitation behavior of Keggin Al13 and Al30 polymers in polyaluminum solutions

The hydrolysis/precipitation behaviors of Al³⁺, Al₁₃ and Al₃₀ under conditions typical for flocculation in water treatment were investigated by studying the particulates' size development, charge characteristics, chemical species and speciation transformation of coagulant hydrolysis precipitates. The optimal pH conditions for hydrolysis precipitates formation for AlCl₃, PAC_Al13 and PAC_Al30 were 6.5–7.5, 8.5–9.5, and 7.5–9.5, respectively. The precipitates' formation rate increased with the increase in dosage, and the relative rates were AlCl₃ ? PAC_Al30 > PAC_Al13. The precipitates' size increased when the dosage increased from 50 μM to 200 μM, but it decreased when the dosage increased to 800 μM. The Zeta potential of coagulant hydrolysis precipitates decreased with the increase in pH for the three coagulants. The iso-electric points of the freshly formed precipitates for AlCl₃, PAC_Al13 and PAC_Al30 were 7.3, 9.6 and 9.2, respectively. The Zeta potentials of AlCl₃ hydrolysis precipitates were lower than those of PAC_Al13 and PAC_Al30 when pH > 5.0. The Zeta potential of PAC_Al30 hydrolysis precipitates was higher than that of PAC_Al13 at the acidic side, but lower at the alkaline side. The dosage had no obvious effect on the Zeta potential of hydrolysis precipitates under fixed pH conditions. The increase in Zeta potential with the increase in dosage under uncontrolled pH conditions was due to the pH depression caused by coagulant addition. Al–Ferron research indicated that the hydrolysis precipitates of AlCl₃ were composed of amorphous Al(OH)₃ precipitates, but those of PAC_Al13 and PAC_Al30 were composed of aggregates of Al₁₃ and Al₃₀, respectively. Al³⁺ was the most un-stable species in coagulants, and its hydrolysis was remarkably influenced by solution pH. Al₁₃ and Al₃₀ species were very stable, and solution pH and aging had little effect on the chemical species of their hydrolysis products. The research method involving coagulant hydrolysis precipitates based on Al–Ferron reaction kinetics was studied in detail. The Al species classification based on complex reaction kinetic of hydrolysis precipitates and Ferron reagent was different from that measured in a conventional coagulant assay using the Al–Ferron method. The chemical composition of Al_a, Al_b and Al_c depended on coagulant and solution pH. The Al_b measured in the current case was different from Keggin Al₁₃, and the high Al_b content in the AlCl₃ hydrolysis precipitates could not used as testimony that most of the Al³⁺ was converted to highly charged Al₁₃ species during AlCl₃ coagulation.     

Pristine/magnesium-loaded biochar and ZVI affect rice grain arsenic speciation and cadmium accumulation through different pathways in an alkaline paddy soil

Cadmium(Cd)and arsenic(As)co-contamination has threatened rice production and food safety.It is challenging to mitigate Cd and As contamination in rice simultaneously due to their opposite geochemical behaviors.Mg-loaded biochar with outstanding adsorption ca-pacity for As and Cd was used for the first time to remediate Cd/As contaminated paddy soils.In addition,the effect of zero-valent iron(ZVI)on grain As speciation accumulation in alkaline paddy soils was first investigated.The effect of rice straw biochar(SC),magnesium-loaded rice straw biochar(Mg/SC),and ZVI on concentrations of Cd and As speciation in soil porewater and their accumulation in rice tissues was investigated in a pot experiment.Addi-tion of SC,Mg/SC and ZVI to soil reduced Cd concentrations in rice grain by 46.1％,90.3％and 100％,and inorganic As(iAs)by 35.4％,33.1％and 29.1％,respectively,and reduced Cd con-centrations in porewater by 74.3％,96.5％and 96.2％,respectively.Reductions of 51.6％and 87.7％in porewater iAs concentrations were observed with Mg/SC and ZVI amendments,but not with SC.Dimethylarsinic acid(DMA)concentrations in porewater and grain increased by a factor of 4.9 and 3.3,respectively,with ZVI amendment.The three amendments affected grain concentrations of iAs,DMA and Cd mainly by modulating their translocation within plant and the levels of As(Ⅲ),silicon,dissolved organic carbon,iron or Cd in porewater.All three amendments(SC,Mg/SC and ZVI)have the potential to simultaneously mitigate Cd and iAs accumulation in rice grain,although the pathways are different.