基于氮掺杂碳量子点的制备及其对Hg2+的响应

以乙二胺和抗坏血酸为原料,通过一步水热法制备了水溶性的氮掺杂碳量子点(N-CQDs).研究了N-CQDs的形貌特征、光学性能和应用分析.表征结果说明,N-CQDs形态为均匀分散的球形,有明显的晶格条纹,抗光漂白性能良好,表面富有含氧官能团,具有良好的水溶性.此外发现N-CQDs还具有优良的荧光性能和荧光稳定性,量子产率可以高达12.29%.分析得出,Hg²⁺对N-CQDs在1.0—120μmol·L^-1范围内有一定的猝灭效应,可作为Hg²⁺的荧光探针,检出限达230 nmol·L^-1.     

黄麻固定化漆酶去除水中Cd2+和刚果红

本文通过酶固定化技术合成漆酶-黄麻复合材料(L-SJ)，以Cd²⁺和刚果红(CR)为模型污染物，通过批处理法研究了黄麻和复合材料对Cd²⁺和CR的等温去除规律，考察了漆酶浓度、温度、pH和离子强度对Cd²⁺和CR去除的影响，并结合红外光谱图探讨其去除机制.研究发现，黄麻和复合材料对Cd²⁺和CR的去除曲线均符合Langmuir等温吸附模型，复合材料对Cd²⁺的去除高于黄麻，增大约1.71—1.96倍，但降低了对CR的去除.黄麻与复合材料对Cd²⁺的去除均表现为放热反应；随pH的增大，黄麻对Cd²⁺的去除先增大后趋于平稳，而复合材料则不断增大；随离子强度的增大，黄麻与复合材料对Cd²⁺的去除不断下降.黄麻与复合材料对CR的去除随温度、离子强度的升高而增大，随pH的增大呈现先增加后降低的趋势.漆酶效能实验发现，NaOH预处理、戊二醛改性和漆酶负载均增大了复合材料对Cd²⁺的去除，NaOH预处理和...     

Ca2+添加对微生物矿化固结Cd2+的影响

微生物诱导碳酸盐沉淀(MICP)可将游离的重金属离子转化为稳定的矿化物,在修复土壤重金属污染方面具有广阔的应用前景.本研究从铜陵矿区周边土壤中筛选得到1株产脲酶且耐镉矿化菌株CZW-1,16S rDNA鉴定为芽孢杆菌(Bacillus sp.),并将其利用于添加外源Ca²⁺的矿化固结Cd²⁺实验中.通过扫描电镜(SEM)、傅立叶红外光谱(FT-IR)以及X射线衍射(XRD)对矿化产物进行表征和分析.结果表明,添加一定浓度的Ca²⁺可促进细菌的生长,其最佳浓度为20 mmol·L^-1.且Ca²⁺的添加可提高细菌的最小抑制浓度和促进脲酶活性,提高对Cd²⁺的矿化率,加钙前后的矿化率由68.93%提高到75.95%.通过对矿化物的定性分析,可知加钙前后的矿物沉淀由单一CdCO₃变为CdCO₃和CaCO₃的复合沉淀,其表面也由严密紧实变成填满了小颗粒CdCO₃的多孔状.     

Fe2+耦合热活化过硫酸盐降解土壤中四溴双酚A

有效降解和去除土壤中四溴双酚A(TBBPA)是土壤环境化学研究热点.本文研究了Fe²⁺耦合热活化过硫酸盐体系(Fe²⁺/热/PS)对土壤中TBBPA的降解,并考察温度、Fe²⁺始浓度、PS浓度、初始pH值、无机阴离子(Cl^-、HCO₃^-)浓度以及金属离子(Cu²⁺、Zn²⁺、Ni²⁺)浓度的影响.结果表明,Fe²⁺/热/PS降解TBBPA的效果远高于同等条件下单一热活化和Fe²⁺活化的情况;提高温度和PS浓度能够促进土壤TBBPA的降解;而过量的亚铁离子会导致TBBPA去除率下降,Fe²⁺与PS的最佳摩尔比为0.5:1;Fe²⁺耦合热活化PS体系具有较宽的pH应用范围,在酸性条件下更有利于降解;温度55℃、Fe²⁺浓度25 mmol·L^-1、PS浓度50 mmo...     

城市森林大气PM2.5中水溶性无机离子沉降特征

森林被誉为"地球之肺",在防霾治污方面有其独特不可替代的作用,不同树种沉降PM_2.5的功能有很大差别.本文选取代表性城市森林——奥林匹克森林公园为研究对象,设置垂直监测塔观测大气PM_2.5的浓度垂直分布,以考察不同季节城市森林对PM_2.5中各组分的影响.在冬季、春季和夏季各采集PM_2.5样品,分析并计算PM_2.5中Na⁺、NH₄⁺、K⁺、Mg2⁺、Ca2⁺、Cl^-、NO₃^-和SO₄^2-等典型水溶性无机离子的浓度.结果表明,PM_2.5中水溶性无机离子总浓度呈规律性变化特征:冬季((56.90±27.38)μg·m-3)>春季((46.69±12.24)μg·m^-3)>夏季((23.16±8.75)μg·m^-3).其中SO₄^2-和NO₃^-浓度和占PM_2.5主要水溶性无机离子总浓度的50%以上.3个季节中,除冬季外,在春季和夏季,8种离子有明显的垂直方向上的沉降,夏季的沉降速率高于春季,但是春季由于大气颗粒物浓度高,沉降通量高于夏季.NO₃^-和SO₄^2-垂直方向的沉降量在所有可溶性无机离子中最高.植被密度、叶面积指数、气象条件等因素对于PM_2.5的沉降特征有明显影响.     

乌鲁木齐市米东区大气降水的化学特征及来源分析

为研究乌鲁木齐市米东区大气降水中的化学组分特征及来源,对2017—2019年降水中主要离子浓度及来源进行了分析。研究结果显示,米东区2017—2019年降水的雨量加权pH年均值为7.95,雨量加权平均电导率年均值为16.15 mS·m^-1,雨量加权平均总离子浓度为72.75—95.89μeq·L^-1,年均浓度为81.93μeq·L^-1。降水中各离子的雨量加权平均浓度顺序为SO₄^2->Ca²⁺>C^l->Na+>NO₃^->NH₄⁺>K⁺>Mg²⁺>F^-,浓度最高的阴、阳离子分别为SO₄^2-(29.01μeq·L^-1)、Ca2+(21.91μeq·L^-1),二者对总离子浓度的贡献分别为35.41%、26.74%。总离子浓度按季节排序为冬季>夏季>秋季>春季。[SO₄^2-/NO₃^-]平均值为7.51,SO₄^2-对雨水酸度的贡献率逐渐减弱,NO₃^-的贡献率逐年增加,降雨的酸化类型为硫酸型,但具有逐步向硝酸型转变的趋势。中和降水中酸性组分的主要碱性离子为连续3年占比最高且稳中有升的Ca²⁺离子。Ca²⁺、Mg²⁺、Na⁺、Cl^-、SO₄^2-、NO₃^-之间存在着较为显著的相关性,说明上述离子有相似的来源并形成化合物共同存在。Ca²⁺在大气中优先与SO₄^2-、NO₃^-结合,且Ca²⁺对雨水酸性的中和贡献率大于NH₄⁺,表明乌鲁木齐市米东区大气降水中可能存在以CaSO₄和Ca(NO₃)₂为主的化学物质。     

安阳市夏季道路积尘水溶性离子污染特征及来源分析

为了解安阳市夏季道路积尘水溶性离子污染特征及来源，于2020年5月使用手持式便携吸尘器采集70个城市道路积尘样品，经离子色谱仪测定其中10种水溶性离子(F^-、Cl^-、NO₂^-、NO₃^-、SO₄^2-、K⁺、Na⁺、Ca²⁺、Mg²⁺、NH₄⁺)，用比值分析法和相关性分析法分析其污染特征，结合地理统计分析和正定矩阵模型判断其主要来源.结果表明，Ca²⁺、SO₄^2-、NO₃^-、Cl^-、K⁺在安阳市道路积尘水溶性离子中占比较大，其中Ca²⁺占比最高，SO₄^2-和NO_...     

氮改性对生物炭理化性质的影响及其对废水中铜离子的吸附特性

原状生物炭对废水中污染物的去除效果有限,改性是提高其吸附能力的重要途径.本文以水稻秸秆为对象,尿素为改性剂,在700℃无氧热解条件下分别制备了原状秸秆生物炭（RSBC）和氮改性秸秆生物炭（N-RSBC）,采用扫描电子显微镜（SEM）、比表面积分析仪（BET）、元素分析仪（EA）、Zeta电位、X射线衍射（XRD）、傅里叶红外光谱（FTIR）以及X射线光电子能谱（XPS）对RSBC和N-RSBC的形貌、比表面积、元素组成、矿物类型和官能团进行表征,考察溶液初始pH值、离子类型和离子强度对生物炭吸附Cu²⁺的影响,并结合吸附等温线和吸附动力学实验、吸附后表征结果探究生物炭对废水中Cu²⁺的吸附性能和机理.结果表明,氮改性导致了生物炭的比表面积和孔体积的降低,而生物炭的官能团类型却更加丰富,特别是含氮官能团.当溶液初始pH值从2.0增加到6.0,生物炭对于Cu²⁺的去除率逐渐增加.对RSBC而言,Na⁺、K⁺、Ca²⁺、Mg2+的存在能略微增加其对Cu^...     

长河流域矿区地表水水化学特征及驱动因子分析

为了研究晋城市长河流域采煤区地表水水质情况、查清其水化学特征,明晰其影响因素及主要离子来源.现场采集了地表水水样9组,采用数理统计方法分析水化学特征,运用Piper三线图分析水化学类型,通过Gibbs图和离子相关分析等方法探讨了地表水主要离子的来源及其影响因素.结果表明,研究区地表水TDS为126—604 mg·L^-1,平均值为344.11 mg·L^-1;pH值为7.43—8.17,平均值为7.79,属于弱碱性水.地表水阳离子以Ca²⁺和Mg²⁺为主,阴离子主要是HCO₃^-,水化学类型为HCO₃^-Mg.通过主要离子的相关性分析可知,TDS与Na⁺、K⁺、HCO₃^-、SO₄^-2和Cl^-都存在显著的正相关性,这些离子对TDS都有贡献.HCO₃<...     

g-C3N4-MoS2/WSe2自偏压系统构建与不同类型污染物同时去除性能研究

由于工业化进程的不断推进,染料与重金属废水被非法排入自然水体,水体污染问题日益严峻.为实现两种污染物的同时去除,本文通过调控合成MoS₂/WSe₂（MW）异质结复合催化材料,提高其催化活性.黑暗条件下,以MoS₂、WSe₂以及MW为阳极材料,g-C₃N₄为阴极材料组建自偏压燃料电池系统,实现在降解有机染料的同时,去除水体中的重金属离子.通过调控参数,探究影响染料与重金属去除的因素.研究表明,影响重金属和有机染料去除效果的因素有pH、电解质溶液浓度、重金属溶液浓度.当溶液pH=5,电解质溶液浓度为0.1 mol·L^-1,铜离子浓度为4 mg·L^-1时,重金属的去除率为64.3%.当溶液pH=5,电解质溶液浓度为0.2 mol·L^-1,铜离子浓度为2 mg·L^-1时,有机染料罗丹明B的去除率为99.5%.该系统在无外加光照条件下,实现不同类型污染物同时去除,并产生约240 ...     

Selective recovery of Cu2+ and Ni2+ from wastewater using bioelectrochemical system

As the bioelectrochemical system, the microbial fuel cell (MFC) and the microbial electrolysis cell (MEC) were developed to selectively recover Cu²⁺ and Ni²⁺ ions from wastewater. The wastewater was treated in the cathode chambers of the system, in which Cu²⁺ and Ni²⁺ ions were removed by using the MFC and the MEC, respectively. At an initial Cu²⁺ concentration of 500 mg·L^-1, removal efficiencies of Cu²⁺ increased from 97.0%±1.8% to 99.0%±0.3% with the initial Ni²⁺ concentrations from 250 to 1000 mg·L^-1, and maximum power densities increased from 3.1±0.5 to 5.4±0.6 W·m^-3. The Ni²⁺ removal mass in the MEC increased from 6.8±0.2 to 20.5±1.5 mg with the increase of Ni²⁺ concentrations. At an initial Ni²⁺ concentration of 500 mg·L^-1, Cu²⁺ removal efficiencies decreased from 99.1%±0.3% to 74.2%±3.8% with the initial Cu²⁺ concentrations from 250 to 1000 mg·L^-1, and maximum power densities increased from 3.0±0.1 to 6.3±1.2 W·m^-3. Subsequently, the Ni²⁺ removal efficiencies decreased from 96.9%±3.1% to 73.3%±5.4%. The results clearly demonstrated the feasibility of selective recovery of Cu²⁺ and Ni²⁺ from the wastewater using the bioelectrochemical system.     

Effective removal of Cd2+ and Pb2+ pollutants from wastewater by dielectrophoresis-assisted adsorption

Dielectrophoresis (DEP) process could enhance the removal the Cd²⁺ and Pb²⁺ with less absorbent. The removal rates of both Cd²⁺ and Pb²⁺ increased with the increase of voltage. The overall removal rate of Cd²⁺ and Pb²⁺ in the binary system is higher than that of Cd²⁺ or Pb²⁺ in the single system. DEP could cause considerable changes of the bentonite particles in both surface morphology and microstructure. Dielectrophoresis (DEP) was combined with adsorption (ADS) to simultaneously and effectively remove Cd²⁺ and Pb²⁺ species from aqueous solution. To implement the process, bentonite particles of submicro-meter size were used to first adsorb the heavy metal ions. These particles were subsequently trapped and removed by DEP. The effects of the adsorbent dosage, DEP cell voltage and the capture pool numbers on the removal rate were investigated in batch processes, which allowed us to determine the optimal experimental conditions. The high removal efficiency, 97.3% and 99.9% for Cd²⁺ and Pb²⁺, respectively, were achieved when the ions are coexisting in the system. The microstructure of bentonite particles before and after ADS/DEP was examined by scanning electron microscopy. Our results suggest that the dielectrophoresis-assisted adsorption method has a high capability to remove the heavy metals from wastewater.     

水环境中天然有机物对纳米颗粒吸附铅和镉的不同作用

为阐明天然有机物(NOM)在纳米颗粒(NPs)吸附重金属中的作用,研究了蛋白质(牛血清白蛋白,BSA)、碳水化合物(海藻酸钠,NaAlg)和腐殖酸(HA)对二氧化钛纳米颗粒(TNPs)和氧化铈纳米颗粒(CNPs)聚集沉降和吸附Cd²⁺和Pb²⁺的影响.结果表明,当Pb²⁺和Cd²⁺在20—120 mg·L-1范围内,HA和NaAlg显著促进了TNPs和CNPs对这些金属离子的吸附(P<0.05),而BSA对这些金属吸附的影响甚微.TNPs-HA和TNPs-NaAlg对Pb²⁺的吸附分别提高了14%—41%和16%—57%,对Cd²⁺的吸附分别提高了12%—112%和22%—143%.与CNPs相比,CNPs-HA和CNPs-NaAlg对Pb²⁺的吸附增加了21%—71%和23%—65%,对Cd²⁺的吸附增加了26%—45%和45%—91%.并且NPs和NPs-NOM对Pb²⁺和Cd²⁺的吸附符合Freundlich吸附模型.离子强度的增加抑制了NPs-HA/NaAlg和NPs对Pb²⁺和Cd²⁺的吸附,而pH的增加对NPs-HA/NaAlg和NPs吸附Pb²⁺和Cd²⁺起促进作用.     

Label-free colorimetric nanosensor with improved sensitivity for Pb2+ in water by using a truncated 8–17 DNAzyme

• Unmodified-AuNP based, colorimetric nanosensor was constructed for Pb²⁺ detection. • 5-nucleotide truncation in DNAzyme made complete substrate detachment upon Pb²⁺. • Ultrasensitive and selective detection of Lead (II) was achieved with 0.2×10^-9 mol/L LOD. Water pollution accidents, such as the Flint water crisis in the United States, caused by lead contamination have raised concern on the safety of drinking water distribution systems. Thus, the routine monitoring of lead in water is highly required and demands efficient, sensitive, cost-effective, and reliable lead detection methods. This study reports a label-free colorimetric nanosensor that uses unmodified gold nanoparticles (AuNPs) as indicators to enable rapid and ultra-sensitive detection of lead in environmental water. The 8–17 DNAzyme was truncated in this study to facilitate the detachment of single-stranded DNA fragments after substrate cleavage in the presence of Pb²⁺. The detached fragments were adsorbed over AuNPs and protected against salt concentration-induced aggregation. Accordingly, high Pb²⁺ would result in rapid color change from blue to pink. The established sensing principle achieved a sensitive limit of detection of 0.2×10^-9 mol/L Pb²⁺, with a linear working range of two orders of magnitude from 0.5×10^-9 mol/L to 5×10^-9 mol/L. The selectivity of the nanosensor was demonstrated by evaluating the interfering metal ions. The developed nanosensor can serve as a substitute for the rapid analysis and monitoring of trace lead levels under the drinking water distribution system and even other environmental water samples.     

Immobilization of Cu2+, Zn2+, Pb2+, and Cd2+ during geopolymerization

The present research explored the application of geopolymerization for the immobilization and solidification of heavy metal added into metakaolinte. The compressive strength of geopolymers was controlled by the dosage of heavy metal cations, and geopolymers have a toleration limit for heavy metals. The influence of alkaline activator dosage and type on the heavy metal ion immobilization efficiency of metakaolinte-based geopolymer was investigated. A geopolymer with the highest heavy metal immobilization efficiency was identified to occur at an intermediate Na₂SiO₃ dosage and the metal immobilization efficiency showed an orderly increase with the increasing Na⁺ dosage. Geopolymers with and without heavy metals were analyzed by the X-ray powder diffraction (XRD) and Fourier transform infrared (FTIR) spectroscopy. No crystalline phase containing heavy metals was detected in geopolymers with heavy metal, suggesting that the crystalline phase containing heavy metals is not produced or most of the phases incorporating heavy metals are amorphous. FTIR spectroscopy showed that, with increasing heavy metal addition, an increase in NO3- peak intensity was observed, which was accompanied by a decrease in the CO32- peak.     

Mercury removal from flue gas using nitrate as an electron acceptor in a membrane biofilm reactor

Membrane bioreactor achieved mercury removal using nitrate as an electron acceptor. The biological mercury oxidation increased with the increase of oxygen concentration. Ferrous sulfide could make both Hg²⁺ and MeHg transform into HgS-like substances. Nitrate drives mercury oxidation through katE, katG, nar, nir, nor, and nos. Mercury (Hg⁰) is a hazardous air pollutant for its toxicity, and bioaccumulation. This study reported that membrane biofilm reactor achieved mercury removal from flue gas using nitrate as the electron acceptor. Hg⁰ removal efficiency was up to 88.7% in 280 days of operation. Oxygen content in flue gas affected mercury redox reactions, mercury biooxidation and microbial methylation. The biological mercury oxidation increased with the increase of oxygen concentration (2%‒17%), methylation of mercury reduced with the increase of oxygen concentration. The dominant bacteria at oxygen concentration of 2%, 6%, 17%, 21% were Halomonas, Anaerobacillus, Halomonas and Pseudomonas, respectively. The addition of ferrous sulfide could immobilize Hg²⁺ effectively, and make both Hg²⁺ and MeHg transform into HgS-like substances, which could achieve the inhibition effect of methylation, and promote conversion of mercury. The dominant bacteria changed from Halomonas to Planctopirus after FeS addition. Nitrate drives mercury oxidation through katE, katG, nar, nir, nor, and nos for Hg⁰ removal in flue gas.     

Influence of arsanilic acid,Cu2+, PO43− and their interaction on anaerobic digestion of pig manure

The methanogenesis was severely inhibited with 0.46 mM ASA addition.PO₄³⁻ didn’t attenuate the methanogenesis inhibition in the existence of ASA.ASA was transformed to As(III), As(V), MMA and DMA in anaerobic digestion.Cu²⁺ mitigated the methanogenesis inhibition via impeding the degradation of ASA.Arsanilic acid (ASA), copper ion (Cu²⁺) and phosphate (PO₄³⁻) are widely used as feed additives for pigs. Most of these three supplemented feed additives were excreted in feces and urine. Anaerobic digestion is often used for the management of pig manure. However, the interaction of ASA with Cu²⁺ or PO₄³⁻ on anaerobic digestion is still not clear. In this study, the influence of ASA, Cu²⁺, PO₄³⁻ and their interaction on anaerobic digestion of pig manure and the possible mechanisms were investigated. The initial concentrations of ASA, Cu²⁺ and PO₄³⁻ were 0.46 mM, 2 mM and 2 mM in the anaerobic digester, respectively. The methanogenesis was severely inhibited in the assays with only ASA addition, only Cu²⁺ addition and ASA+ PO₄³⁻ addition with the inhibition index of 97.8%, 46.6% and 82.6%, respectively, but the methanogenesis inhibition in the assay with ASA+ Cu²⁺ addition was mitigated with the inhibition index of 39.4%. PO₄³⁻ had no obvious impacts on the degradation of ASA. However, Cu²⁺ addition inhibited the degradation of ASA, mitigating the methanogenesis inhibition. The existence of ASA would inhibit methanogenesis and generate more toxic inorganic arsenic compounds during anaerobic digestion, implying the limitation of anaerobic digestion for ASA- contaminated animal manure. However, the co-existence of ASA and Cu²⁺ could mitigate the inhibition. These results could provide useful information for the management of anaerobic digestion of pig manure containing ASA with Cu²⁺.     

Decomposition of aqueous chlorinated contaminants by UV irradiation with H2O2

In the present study, the decomposition rates of carbon tetrachloride (CCl₄) and 2,4-dichlorophenol (2,4-DCP) in water by the ultraviolet (UV) light irradiation alone and H₂O₂/UV were experimentally investigated. The detailed experimental studies have been conducted for examining treatment capacities of the two different ultraviolet light sources (low and medium pressure Hg arc) in H₂O₂/UV processes. The low or medium UV lamp alone resulted in a 60%–90% decomposition of 2,4-DCP while a slight addition of H₂O₂ resulted in a drastic enhancement of the 2,4-DCP decomposition rate. The decomposition rate of 2,4-DCP with the medium pressure UV lamp alone was about 3–6 times greater than the low pressure UV lamp alone. In the direct photolysis of aqueous CCl₄, the medium pressure UV lamp had advantage over the low pressure UV lamp because the molar extinction coefficient of CCl₄ at shorter wavelength (210–220 nm) is about 20 to 50 times higher than that at 254 nm. However, adding H₂O₂ to the medium pressure UV lamp system rendered a negative oxidation rate because H₂O₂ acted as a UV absorber being competitive with CCl₄ due to negligible reaction between CCl₄ and OH radicals. The results from the present study indicated significant influence of the photochemical properties of the target contaminants on the photochemical treatment characteristics for designing cost-effective UV-based degradation of toxic contaminants.