γ辐照降解水中磺胺嘧啶的研究

实验研究了水中磺胺嘧啶（SD）的γ辐照降解,考察了SD初始浓度、溶液pH值,以及联合H2O2、Fenton试剂对其辐照降解的影响.结果表明：γ辐照可有效降解水中SD,低浓度SD在酸性条件下的辐照降解更为显著,降解过程遵循准一级反应动力学模型.添加H2O2可在一定程度上促进SD的γ辐照降解,加入Fenton试剂则显著提升...     

臭氧氧化降解水中磺胺嘧啶的机理研究

环境中残留的抗生素药物对生态环境的危害受到极大关注。研究了臭氧对水中磺胺嘧啶(SD)的降解,考察了溶液pH、臭氧浓度和HC O 3 - 投加量对臭氧降解SD的影响,并对其降解机理进行了分析。结果表明:初始pH、臭氧浓度及HC O 3 - 均对臭氧氧化降解SD过程造成影响,提高pH、增加臭氧浓度和HC O 3 - 投加量均能提高SD降解速率;在SD浓度为30 mg/L、初始pH为9.14、臭氧浓度为10.0 mg/L、HC O 3 - 投加量为100 mg/L时,反应30 min后SD基本被去除,120 min后SD的最终矿化率为39.44%;臭氧降解SD过程基本符合伪一级动力学模型。液相色谱-质谱分析结果显示:臭氧氧化SD过程中,生成中间产物对氨基苯磺酸(C6H7NO3S),经臭氧进一步氧化分解,最终矿化生成CO2。     

水中磺胺甲(噁)唑和磺胺嘧啶的γ辐照降解研究

文章研究了水溶液中磺胺甲啊恶唑(SMX)和磺胺嘧啶(SD)的γ射线辐照降解,考察了吸收剂量、初始浓度、溶解氧和pH值条件对SMX和SD降解的影响。结果表明,γ辐照可有效降解水中的SMX和SD,其降解率和矿化程度随吸收剂量的增加而升高;较低的初始浓度和中性溶液条件有利于SMX和SD的辐照降解;溶解氧可使降解受到一定的抑制,强酸和强碱环境均不利于反应的进行。在pH为6.5的条件下,初始浓度为5 mg/L的SMX和SD溶液分别受到5 kGy和1.5 kGy的辐射照射时,SMX和SD被完全降解转化,研究结果可为水体中抗生素的辐照降解提供技术参考。     

毫米级根际微域磺胺嘧啶的降解动态研究

采用特制根际箱,研究了玉米根际效应作用下磺胺嘧啶在土壤中的降解动态.在空间上将根-土界面(0~5 mm)细化到1 mm,箱内磺胺嘧啶剂量分别设为1 mg·kg-1和5 mg·kg-1,分别在出苗后第20、40和60 d取样,并将磺胺嘧啶降解率与根-土界面4种有机酸含量进行回归分析,从而得出影响磺胺嘧啶在根际土壤降解的关键因素.结果表明,种植作物可有效促进磺胺嘧啶的降解,且磺胺嘧啶的最大消减水平发生在距离根室3 mm的近根区,降解顺序依次为:近根际根室远根际.通过对不同剂量磺胺嘧啶胁迫下有机酸响应的相关分析发现,苹果酸和乙酸是影响磺胺嘧啶在根际土壤中降解的关键因素之一.     

以天然电气石为催化剂的电Fenton体系降解磺胺二甲基嘧啶的工艺研究

磺胺二甲基嘧啶(SMT)是一种抗菌效果较好的抗生素,被广泛用于人体和牲畜的疾病治疗中,在世界范围内已具有较大规模的应用。但由于其在动物体内不能被完全吸收,因此会随着粪便排出,污染自然界水体。以天然电气石作为催化剂构建了电Fenton反应体系,其过氧化氢(H₂O₂)由阴极原位生成。探究了不同pH、SMT初始浓度、温度、电流密度、电气石投加量对SMT降解的影响。     

磺胺二甲基嘧啶在过硫酸盐存在下的辐照降解研究

本研究对磺胺二甲基嘧啶(SMT)在不同条件下的辐照降解进行了研究.SMT(20 mg·L~(-1),约0.072 mmol·L~(-1))在外加过硫酸根浓度为0、1、2、4、10和20 mmol·L~(-1)条件下分别进行辐照,发现伽马辐照可有效去除水中的SMT,并可极大地促进溶液TOC的去除,过硫酸盐与伽马辐照联合作用表现出明显的协同效应.在本研究中,各条件下的辐照降解反应均符合准一级反应动力学.在外加过硫酸盐的条件下,溶液的矿化度可以得到极大的提高,当吸收剂量为1 k Gy时,其矿化度由3.5%提高到22.8%,当吸收剂量为5 k Gy时,矿化度由14.1%提高到70.1%.在辐解后的溶液中,利用IC检测到硫酸根离子(SO_4~(2-))、甲酸根离子(HCOO~-)和乙酸根离子(CH_3COO~-)3种离子的存在,一部分中间产物通过GC-MS检测得到,常见的含氮离子(NO_2~-、NO_3~-和NH_4~++)并未在溶液中检测到.同时,本研究还深入探讨了SMT辐照降解机理和降解途径.     

抗生素磺胺嘧啶和磺胺甲恶唑在土壤中的淋溶行为研究

农业生产中畜禽粪污还田会将残留的抗生素带入农田土壤,并能通过淋溶作用迁移至深层土壤最终进入地下水. 该研究采用模拟土壤柱淋溶试验方法,研究了2种磺胺类抗生素——磺胺嘧啶(sulfadiazine,SDZ)和磺胺甲恶唑(sulfamethoxazole,SMX)在农田土壤中的淋溶行为,以及表层土抗生素含量、淋溶液pH和有机质对各土柱剖面SDZ和SMX残留水平的影响. 结果表明:①不同表层土抗生素含量下,SDZ和SMX在供试土壤中均呈向下迁移的趋势,但淋溶结束后上层土壤中二者含量明显高于下层,土柱各层抗生素的含量随表层土抗生素含量的增加而增加. ②淋溶液pH为3.00和5.00时,各层土壤中SDZ和SMX的含量均高于淋溶液pH为7.00时. 淋溶液pH较高时两种磺胺类抗生素多以阴离子形态存在,会与带负电荷的土壤颗粒产生静电斥力而易于向下迁移;随着淋溶液pH的降低,两种磺胺类抗生素阴离子形态占比减少,上层土壤中保留的抗生素含量变高,向下迁移的能力减弱. ③粪便添加组上层土壤中SDZ和SMX的含量明显高于未添加组,抗生素向下迁移的能力减弱,这与有机质的添加使得上层土柱吸附能力增强有关. 通过模型模拟,SDZ和SMX的地下水污染指数分别为3.50和4.45,均大于2.8,表明在供试土壤中这2种磺胺类抗生素的淋溶迁移性较强. 研究显示,淋溶试验结果与模型模拟结果一致,表明SDZ和SMX对地下水存在潜在污染风险.      

碳纳米管高效活化高铁酸盐降解水中磺胺二甲基嘧啶的机理研究

过往的研究表明,引入均相/非均相还原剂或额外能量来诱导Fe(Ⅵ)形成铁活性中间体(Fe(Ⅳ和Fe(Ⅴ))对水中污染物进行处理会导致Fe(Ⅵ)的利用率低,需要创新的活化策略.基于此,本文采用碳纳米管(CNT)/Fe(Ⅵ)体系对水中磺胺二甲基嘧啶(SMT)进行降解,并研究体系的作用机理和SMT的降解机制.研究发现,CNT可以介导从SMT到Fe(Ⅵ)的直接电子转移,CNT在体系中起电子介体而不是电子供体的作用.在50 mg·L^-1 CNT和100.0μmol·L^-1 Fe(Ⅵ)的作用下,5.0μmol·L^-1 SMT能够在10 min内实现完全降解,它在该体系中的转化途径主要包括苯胺部分的氧化、磺酰胺键的断裂和Smiles型重排.另外,CNT/Fe(Ⅵ)体系在不同天然水体中都有较好的SMT去除率.本研究相关结果为活化Fe(Ⅵ)氧化污染物过程中的电子转移机制提供了新的解释.     

水热法制备BiVO4及其可见光催化降解糖蜜酒精废水

以Bi(NO3)3•5H2O为铋源,NH4VO3为钒源,采用简单的水热法制备了BiVO4 光催化剂,并用X-射线衍射(XRD)、扫描电子显微镜(SEM)、红外光谱(IR)和紫外-可见光漫反射光谱(UV-vis)对产品进行了结构表征。同时,在BiVO4光催化降解糖蜜酒精废水反应中考察了催化剂用量、通氧量、溶液pH值、双氧水用量及光照强度对糖蜜酒精废水脱色率的影响。实验结果表明,水热产品属于单斜晶系BiVO4,其带隙能为2.398 eV,并具有良好的可见光催化活性。当降解经30倍稀释的糖蜜酒精废水,BiVO4添加量为3.0 g•L−1 ,通氧量为120 L•h-1,助氧化剂H2O2添加量为9 %,不改变废水pH值,在400W镝灯离液面11cm照射反应180 min的条件下,糖蜜酒精废水的脱色率为88.60 %,COD去除率为25.84%,而添加5g•L−1的FeSO4•7H2O后其脱色率和COD去除率分别提高到90.90 %和91.26%。单斜晶型BiVO4晶体的可见光催化糖蜜酒精废水过程符合一级动力学反应。     

中药渣生物炭对磺胺甲基嘧啶的吸附及机理研究

以传统中药-黄芪废渣为原料,分别在200℃、400℃、500℃、600℃和700℃的厌氧氛围下热解制备生物炭材料（BC200、BC400、BC500、BC600和BC700）,并利用BET比表面积分析、FTIR光谱分析、扫描电子显微镜等方法对其进行表征,同时考察不同投加量、吸附时间、初始浓度和pH值下生物炭对磺胺甲基嘧啶的吸附特征.结果表明,随制备温度的升高,生物炭的表面积及吸附性能也显著增加.相比原状黄芪渣（S_BET=0.42m²/g）,BC700的BET比表面积（S_BET=155.69m²/g）增大370倍,对磺胺甲基嘧啶的吸附容量增加185倍.BC700对磺胺甲基嘧啶的等温吸附过程符合Langmuir模型（R²=0.9977）,最大吸附容量为11.96mg/g,吸附反应过程满足准二级动力学方程（R²>0.994）,且为化学吸附.同时随着溶液初始pH值和投加量的升高,生物炭的吸附容量先增大后减小,最佳吸附pH值为4.     

Fabrication and photoelectrocatalytic properties of nanocrystalline monoclinic BiVO4 thin-film electrode

Monoclinic bismuth vanadate(BiVO4) thin film was fabricated on indium-tin oxide glass from an amorphous heteronuclear complex via dip-coating.After annealation at 400,500,and 600°C,the thin films were characterized by X-ray diffraction,field emission scanning electron microscopy,X-ray photoelectron spectroscopy,and UV-Vis spectrophotometry.The BiVO4 particles on the ITO glass surface had a monoclinic structure.The UV-Visible diffuse reflection spectra showed the BiVO4 thin film had photoabsorption propertie...     

Bi/BiVO4/NiFe-LDH heterostructures with enhanced photoelectrochemical performance for streptomycin detection

Streptomycin (STR) plays an essential role in bacterial infection treatments. Selectivity and sensitivity of photoelectrochemical (PEC) sensors are the two most important parameters, which can be measured using the photosensitivity of its active material. We prepared a novel PEC sensor to detect STR using Bi/BiVO₄/LDH (layered double hydroxides) heterostructures as an active material, which is photoactive in the visible light wavelength range. The simultaneous presence of LDH and Bi/BiVO₄ enhanced the material photocurrent response, which was linear to the STR concentrations in the 0.01–500 nmol/L range. The STR detection limit by this sensor was 0.0042 nmol/L. Our novel PEC-based sensing strategy includes using an ultra-sensitive and highly selective sensor for STR detection. Additionally, the two-pot synthesis of Bi/BiVO₄/LDH developed in this work is environmentally friendly.     

Enhancement of photocatalytic efficiency by in situ fabrication of BiOBr/BiVO4 surface junctions

Surface junctions between Bi OBr and BiVO_4 were synthesized. The BiOBr/BiVO_4 with 1 wt.%of Bi OBr exhibited the highest photocatalytic activity in the degradation of Rh B under visible-light irradiation. It was found that the highly efficient adsorption of Rh B molecules via the electrostatic attraction between Br-and cationic \N(Et)_2 group played a key role for the high photocatalytic activities of BiOBr/BiVO_4. This efficient adsorption promoted the N-deethylation of Rh B and thus accelerated the photocatalytic degradation of Rh B.Moreover, the metal-to-metal charge transfer(MMCT) mechanism was proposed, which revealed the concrete path paved with Bi–O–Bi chains for the carrier migration in BiOBr/BiVO_4. The interaction between photoexcited Rh B* and the Bi~(3+) in BiVO_4 provided the driving force for the migration of photo-generated carriers along the Bi–O–Bi chains. This work has not only demonstrated the important role of efficient adsorption in the photocatalytic degradation of organic contaminants, but also developed a facile strategy to improve the efficiency of photocatalysts.     

One-pot molten salt method for constructing CdS/C3N4 nanojunctions with highly enhanced photocatalytic performance for hydrogen evolution reaction

The construction of heterojunction photocatalysts for efficiently utilizing solar energy has attracted considerable attention to solve the energy crisis and reduce environmental pollution. In this study, we use the energy released from an easily-occurred exothermic chemical reaction to serve as the drive force to trigger the formation of Cd S and C₃N₄ nanocomposites which are successfully fabricated with cadmium nitrate and thiourea without addition of any solvents and prot...     

羟基化锌催化臭氧氧化去除水中痕量磺胺嘧啶

以实验室制备的羟基化锌(ZnOOH)为催化剂,研究了其催化臭氧化去除水中痕量磺胺嘧啶(SD)的效能,通过研究叔丁醇对催化效果的影响,推断了催化反应机理,探讨了臭氧投加量、水质因素、催化剂投加量和使用次数对催化性能的影响因素.结果表明,ZnOOH对臭氧氧化水中的SD有较强的催化活性.催化剂表面结合的羟基基团有利于催化反应.在优化的实验条件下,蒸馏水中反应30min时,催化臭氧化比单独臭氧化对SD的去除率提高了47.7%.催化过程遵循自由基反应机理,SD的去除效果随催化剂投加量的增加而提高,催化剂在重复使用后催化效果基本不变,水中的氯离子可以明显降低催化剂的活性,偏碱性条件下,催化效果更佳.     

In situ preparation of g-C3N4/polyaniline hybrid composites with enhanced visible-light photocatalytic performance

The graphic carbon nitride/polyaniline (g-C₃N₄/PANI) hybrid composites were successfully synthesized by a facile in situ polymerization process under ice water bath. The photocatalytic activities of the g-C₃N₄/PANI composites were evaluated by using oxytetracycline (OTC) as model pollutants. The optimal g-C₃N₄/PANI composite (5%PANI: the g-C₃N₄/PANI hybrid with 5 wt.% of PANI) showed an enhancement degradation rate of 5-fold compared to that of conventional g-C₃N₄ under simulated-sunlight irradiation. In addition, the 5%PANI demonstrate significantly photocatalytic evolution H₂ rate (163.2 μmol/(g?hr)) under the visible light irradiation. Furthermore, based on the results of optical performance and electrochemical testing, a possible mechanism was proposed, indicating that the incorporation of PANI into the traditional g-C₃N₄ can effectively tune the electronic structures, improve the photo-generated electrons-holes separation and enhance extensive absorption of visible light. Such a g-C₃N₄/PANI hybrid nanocomposites could be envisaged to possess great potentials in practical wastewater treatment and water splitting.     

亚临界水处理模拟有机-矿质复合体形成机制探讨

为模拟地质吸附剂中的有机质矿化腐殖化及有机-矿质复合体的形成过程,采用亚临界水处理技术,通过控制压力反应釜的温度、压力和反应时间对商用腐殖酸、高岭土及有机-矿质复合体进行处理,并通过比表面积全分析、傅里叶红外光谱（FTIR）、特定波长可见吸光度比值（E₄/E₆）、X射线衍射（XRD）和¹³C核磁共振（¹³C-NMR）等表征手段尝试探讨不同处理条件下有机质、粘土矿物及二者复合体的各自变化特征及机制.结果表明,升温增压不仅导致腐殖酸比表面积显著增加,而且分子量变大,芳化度由59.52%增加到70.90%,其主要原因是游离羧基和链烃在升温增压条件下实现了成环、聚合过程,使其结构更加复杂,化学稳定性提高.高岭土在升温增压的过程中脱水,形成结晶更加完整的有序结构.腐殖酸与高岭土形成有机-矿质复合体的过程中存在多重作用,首先高岭土优先选择腐殖酸分子中的芳香组分进行插层,至形成较为致密的内层结构,其次,补丁在外围的游离羧基、烷氧和链式结构在高温高压的作用下成环、聚合形成疏松的外层空间.高岭土、腐殖酸及二者的复合体的变化趋势分别与天然环境中粘土矿物及有机质的矿化腐殖化进程和方向相一致.     

Effect of sulfur source on photocatalytic degradation performance of CdS/MoS2 prepared with one-step hydrothermal synthesis

Cd S/Mo S_2,an extremely efficient photocatalyst,has been extensively used in hydrogen photoproduction and pollutant degradation.Cd S/Mo S_2can be synthesized by a facile one-step hydrothermal process.However,the effect of the sulfur source on the synthesis of Cd S/Mo S_2via one-step hydrothermal methods has seldom been investigated.We report herein a series of one-step hydrothermal preparations of Cd S/Mo S_2using three different sulfur sources:thioacetamide,L-cysteine,and thiourea.The results revealed that the sulfur source strongly affected the crystallization,morphology,elemental composition and ultraviolet(UV)–visible-light-absorption ability of the Cd S/Mo S_2.Among the investigated sulfur sources,thioacetamide provided the highest visible-light absorption ability for Cd S/Mo S_2,with the smallest average particle size and largest surface area,resulting in the highest efficiency in Methylene Blue(MB)degradation.The photocatalytic activity of Cd S/Mo S_2synthesized from the three sulfur sources can be arranged in the following order:thioacetamideL-cysteinethiourea.The reaction rate constants(k)for thioacetamide,L-cysteine,and thiourea were estimated to be 0.0197,0.0140,and 0.0084 min~(-1),respectively.However,thioacetamide may be limited in practical application in terms of its price and toxicity,while L-cysteine is relatively economical,less toxic and exhibited good photocatalytic degradation performance toward MB.     

Enhanced photocatalytic activity of nanotube-like titania by sulfuric acid treatment

IntroductionTiO2 nanotubehaswidelydrawnmuchattentionduetoitslargesurfaceareaandhighphotocatalyticactivity ,becausetheyhavegreatpotentialforsuchapplicationsasenvironmentalpurification ,decompositionofcarbonicacidgas,andgenerationofhydrogengas .Titaniananot…