Mesoporous carbon adsorbents from melamine–formaldehyde resin using nanocasting technique for CO2 adsorption

Mesoporous carbon adsorbents, having high nitrogen content, were synthesized via nanocasting technique with melamine–formaldehyde resin as precursor and mesoporous silica as template. A series of adsorbents were prepared by varying the carbonization temperature from 400 to 700°C. Adsorbents were characterized thoroughly by nitrogen sorption, X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), thermogravimetric analysis (TGA), elemental (CHN) analysis, Fourier transform infrared (FTIR) spectroscopy and Boehm titration. Carbonization temperature controlled the properties of the synthesized adsorbents ranging from surface area to their nitrogen content, which play major role in their application as adsorbents for CO₂ capture. The nanostructure of these materials was confirmed by XRD and TEM. Their nitrogen content decreased with an increase in carbonization temperature while other properties like surface area, pore volume, thermal stability and surface basicity increased with the carbonization temperature. These materials were evaluated for CO₂ adsorption by fixed-bed column adsorption experiments. Adsorbent synthesized at 700°C was found to have the highest surface area and surface basicity along with maximum CO₂ adsorption capacity among the synthesized adsorbents. Breakthrough time and CO₂ equilibrium adsorption capacity were investigated from the breakthrough curves and were found to decrease with increase in adsorption temperature. Adsorption process for carbon adsorbent–CO₂ system was found to be reversible with stable adsorption capacity over four consecutive adsorption–desorption cycles. From three isotherm models used to analyze the equilibrium data, Temkin isotherm model presented a nearly perfect fit implying the heterogeneous adsorbent surface.     

Mesoporous carbon adsorbents from melamine-formaldehyde resin using nanocasting technique for CO2 adsorption

Mesoporous carbon adsorbents, having high nitrogen content, were synthesized via nanocasting technique with melamine–formaldehyde resin as precursor and mesoporous silica as template. A series of adsorbents were prepared by varying the carbonization temperature from 400 to 700°C. Adsorbents were characterized thoroughly by nitrogen sorption, X-ray diffraction(XRD), scanning electron microscopy(SEM), transmission electron microscopy(TEM), thermogravimetric analysis(TGA), elemental(CHN) analysis, Fourier transform infrared(FTIR) spectroscopy and Boehm titration. Carbonization temperature controlled the properties of the synthesized adsorbents ranging from surface area to their nitrogen content, which play major role in their application as adsorbents for CO_2 capture.The nanostructure of these materials was confirmed by XRD and TEM. Their nitrogen content decreased with an increase in carbonization temperature while other properties like surface area, pore volume, thermal stability and surface basicity increased with the carbonization temperature. These materials were evaluated for CO_2 adsorption by fixed-bed column adsorption experiments. Adsorbent synthesized at 700°C was found to have the highest surface area and surface basicity along with maximum CO_2 adsorption capacity among the synthesized adsorbents. Breakthrough time and CO_2 equilibrium adsorption capacity were investigated from the breakthrough curves and were found to decrease with increase in adsorption temperature. Adsorption process for carbon adsorbent–CO_2 system was found to be reversible with stable adsorption capacity over four consecutive adsorption–desorption cycles. From three isotherm models used to analyze the equilibrium data, Temkin isotherm model presented a nearly perfect fit implying the heterogeneous adsorbent surface.     

土壤胡敏素对铜离子的吸附作用及其机理研究

以暗棕壤为供试土壤,研究了不同溶液pH值、离子强度、接触时间、反应温度和初始铜离子(Cu~(2+))浓度条件下,胡敏素对Cu~(2+)的吸附作用;利用扫描电子显微镜(SEM)、X-射线能量色散谱(EDS)、傅立叶变换红外光谱(FTIR)和X-射线光电子能谱(XPS),对胡敏素/胡敏素-Cu~(2+)复合物的表面形貌、元素分布和官能团组成进行了分析;应用延展X-射线吸收精细结构谱(EXAFS),对吸附态Cu~(2+)的局域配位结构进行了表征.结果表明:胡敏素对Cu~(2+)的吸附量随pH值、接触时间、反应温度和Cu~(2+)浓度的增加而增加,但随离子强度的增加而下降;吸附动力学符合准二级动力学方程,而吸附等温线用Langmuir方程的拟合效果较好;吸附过程需要能量,是自发、吸热和自由度增加的缔合反应;吸附Cu~(2+)之后,胡敏素表面产生了团聚现象,表面羧基、羟基、吡啶氮和N—O基团参与了Cu~(2+)的吸附作用,同时吸附态Cu~(2+)是以内层配位形式与胡敏素表面的O/N和C原子结合.     

二氧化钛对地下水中砷硅的吸附及再生回用

二氧化钛(TiO_2)材料作为性能优异的吸附材料被广泛应用于地下水砷(As)的去除中.结果表明,地下水中共存硅离子(Si)会占据TiO_2的吸附位点,从而影响As的吸附及TiO_2材料的再生回用.本文通过同步辐射扩展X射线吸收精细结构(EXAFS)研究了Si对As微观吸附机制的影响,表明Si的存在不会影响As在TiO_2上的吸附构型.衰减全反射傅里叶变换红外光谱(ATR-FTIR)原位研究表明Si在TiO_2表面形成Si单体、低聚体和多聚体,从而竞争As的吸附位点,同时增加TiO_2再生的难度.为了实现TiO_2材料的高效再生,本研究进一步考察了氟化钠(NaF)对TiO_2表面Si的脱附效果,发现NaF可以有效地洗脱Si,再生后的TiO_2吸附性能稳定.ATR-FTIR光谱原位分析发现,NaF的加入可有效脱附TiO_2表面的Si单体和多聚体.当利用NaF和Na OH共同洗脱TiO_2表面的As和Si时,3次循环中As的脱附率为86.8%~100.3%,Si的脱附率为67.9%~82.0%.本研究为地下水砷硅共吸附材料的再生提供了一种有效方法.     

针铁矿-高岭石复合体的表面性质和吸附氟的特性

采用X-射线衍射(XRD)、扫描电镜(SEM)、红外(FT-IR)光谱、质子电位滴定、比表面及微孔分析等方法对针铁矿、高岭石及其复合体的基本性质进行了表征;研究了供试样品对氟的吸附容量及吸附模型.结果表明,在悬浮液体系中,针铁矿可包被在高岭石表面形成二元复合体.复合体的孔径主要分布在0.42 nm和0.61 nm左右,BET表面积为34.08 m2/g,表面分形度D=2.726,质子电荷零点(pHPZNPC)位于5.50～6.50间.初始pH=6.00时,针铁矿对氟的吸附容量(qmax)为4.506 mg/g,高岭石的吸附容量为0.608 mg/g,复合体的吸附容量为3.520 mg/g.用Langmuir和Freundlich方程拟合了针铁矿、高岭石及复合体对氟的等温吸附数据,其中Langmuir方程拟合的相关系数(R2)分别为0.964、0.991和0.799,Freundlich方程拟合的相关系数分别为0.925、0.886和0.995.3种矿物吸附氟的主要机制有阴离子配体交换、表面配位和静电作用;此外,"F-键桥"对复合体吸附氟也有重要贡献.与2种单体的平均值比较,针铁矿-高岭石复合体的孔体积和孔径分布无明显变化,比表面积和表面分形度增加,表面羟基含量和质子电荷量减少,吸附氟的能力增强.针铁矿和高岭石单体对氟的吸附属于单层吸附模式,适合用Langmuir方程拟合;多层吸附模型Freundlich方程可很好地描述复合体对氟的吸附.     

Preliminary investigation of phosphorus adsorption onto two types of iron oxide-organic matter complexes

Iron oxide(FeO)coated by natural organic matter(NOM)is ubiquitous.The associations of minerals with organic matter(OM)significantly changes their surface properties and reactivity,and thus affect the environmental fate of pollutants,including nutrients(e.g.,phosphorus(P)).In this study,ferrihydrite/goethite-humic acid(FH/GE–HA)complexes were prepared and their adsorption characteristics on P at various p H and ionic strength were investigated.The results indicated that the Fe O–OM complexes showed a decreased P adsorption capacity in comparison with bare Fe O.The maximum adsorption capacity(Q_(max))decreased in the order of FH(22.17 mg/g)FH-HA(5.43 mg/g)GE(4.67 mg/g)GE-HA(3.27 mg/g).After coating with HA,the amorphous FH–HA complex still showed higher P adsorption than the crystalline GE–HA complex.The decreased P adsorption observed might be attributed to changes of the Fe O surface charges caused by OM association.The dependence of P adsorption on the specific surface area of adsorbents suggests that the Fe O component in the complexes is still the main contributor for the adsorption surfaces.The P adsorptions on Fe O–HA complexes decreased with increasing initial p H or decreasing initial ionic strength.A strong dependence of P adsorption on ionic strength and p H may demonstrate that outer-sphere complexes between the OM component on the surface and P possibly coexist with inner-sphere surface complexes between the Fe O component and P.Therefore,previous over-emphasis on the contributions of original minerals to P immobilization possibly over-estimates the P loading capacity of soils,especially in humic-rich areas.     

Photocatalytic decomposition of acrylonitrile with N–F codoped TiO2/SiO2 under simulant solar light irradiation

The solid acid catalyst, N–F codoped TiO₂/SiO₂ composite oxide was prepared by a sol–gel method using NH₄F as nitrogen and fluorine source. The prepared materials were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), UV–Visible diffuse reflectance spectroscopy (UV–Vis), ammonia adsorption and temperature-programmed desorption (NH₃-TPD), in situ Fourier transform infrared spectroscopy (FT-IR) and N₂ physical adsorption isotherm. The photocatalytic activity of the catalyst for acrylonitrile degradation was investigated under simulant solar irradiation. The results showed that strong Lewis and Brønsted acid sites appear on the surface of the sample after N–F doping. Systematic investigation showed that the highest photocatalytic activity for acrylonitrile degradation was obtained for samples calcined at 450°C with molar ratio (NH₄F to Ti) of 0.8. The degradation ratio of 71.5% was achieved with the prepared catalyst after 6-min irradiation, demonstrating the effectiveness of photocatalytic degradation of acrylonitrile with N–F codoped TiO₂/SiO₂ composite oxide. The photocatalyst is promising for application under solar light irradiation. Moreover, the intermediates generated after irradiation were verified by gas chromatography–mass spectrometry (GC–MS) analysis and UV–Vis spectroscopy to be simple organic acids with lower toxicity, and the degradation pathway was also proposed for acrylonitrile degradation with the prepared catalyst.     

Synthesis, characterization, and photocatalytic activity of porous La–N–co-doped TiO2 nanotubes for gaseous chlorobenzene oxidation

The photocatalytic oxidation of gaseous chlorobenzene(CB) by the 365 nm-induced photocatalyst La/N–Ti O2, synthesized via a sol–gel and hydrothermal method, was evaluated. Response surface methodology(RSM) was used to model and optimize the conditions for synthesis of the photocatalyst. The optimal photocatalyst was 1.2La/0.5N–Ti O2(0.5) and the effects of La/N on crystalline structure, particle morphology, surface element content, and other structural characteristics were investigated by XRD(X-ray diffraction), TEM(Transmission Electron Microscopy), FTIR(Fourier transform infrared spectroscopy), UV–vis(Ultraviolet–visible spectroscopy), and BET(Brunauer Emmett Teller). Greater surface area and smaller particle size were produced with the co-doped Ti O2 nanotubes than with reference Ti O2. The removal of CB was effective when performed using the synthesized photocatalyst,though it was less efficient at higher initial CB concentrations. Various modified Langmuir-Hinshelwood kinetic models involving the adsorption of chlorobenzene and water on different active sites were evaluated. Fitting results suggested that competitive adsorption caused by water molecules could not be neglected, especially for environments with high relative humidity. The reaction intermediates found after GC–MS(Gas chromatography–mass spectrometry) analysis indicated that most were soluble, low-toxicity, or both. The results demonstrated that the prepared photocatalyst had high activity for VOC(volatile organic compounds) conversion and may be used as a pretreatment prior to biopurification.     

Hg removal from flue gas over different zeolites modified by FeCl3

The elemental mercury removal abilities of three different zeolites (NaA, NaX, HZSM-5) impregnated with iron(III) chloride were studied on a lab-scale fixed-bed reactor. X-ray diffraction, nitrogen adsorption porosimetry, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, and temperature programmed desorption (TPD) analyses were used to investigate the physicochemical properties. Results indicated that the pore structure and active chloride species on the surface of the samples are the key factors for physisorption and oxidation of Hg⁰, respectively. Relatively high surface area and micropore volume are beneficial to efficient mercury adsorption. The active Cl species generated on the surface of the samples were effective oxidants able to convert elemental mercury (Hg⁰) into oxidized mercury (Hg^2 +). The crystallization of NaCl due to the ion exchange effect during the impregnation of NaA and NaX reduced the number of active Cl species on the surface, and restricted the physisorption of Hg⁰. Therefore, the Hg⁰ removal efficiencies of the samples were inhibited. The TPD analysis revealed that the species of mercury on the surface of FeCl₃–HZSM-5 was mainly in the form of mercuric chloride (HgCl₂), while on FeCl₃–NaX and FeCl₃–NaA it was mainly mercuric oxide (HgO).     

聚合氯化铝镁钛的制备及结构表征

为提高铝基复合混凝剂的混凝效果,以AlCl₃、MgCl₂、TiCl₄为原料,通过共聚反应制备出无机复合高分子混凝剂PCAMT（聚合氯化铝镁钛）,并探究其混凝机理.采用Ferron（高铁试剂）逐时络合比色法、红外光谱、X-射线衍射谱图、扫描电镜与能谱分析（SEM-EDS）、Zeta电位对产物的Al形态、结构形貌、组成及混凝机理进行分析.结果表明:①采用单因素试验法获得最佳合成条件,即反应温度为60 ℃,Mg/Al（摩尔比,下同）为0.5,Ti/Al（摩尔比,下同）为0.5,OH/（Al+Mg+Ti）（摩尔比,下同）为0.6.②形态分析表明,反应温度、Mg/Al、Ti/Al,OH/（Al+Mg+Ti）对Al的形态分布均存在影响.随着反应温度的升高,n（Ala）（Ala在Al的水解聚合形态中所占摩尔分数,下同）先减后增,n（Alb）（Alb在Al的水解聚合形态中所占摩尔分数,下同）先增后减,n（Alc）（Alc在Al的水解聚合形态中所占摩尔分数,下同）逐渐减小;随着Mg/Al的增大,n（Ala）先减后增,n（Alb）、n（Alc）为先增后减的趋势;随着Ti/Al的增大,n（Ala）逐渐增加,n（Alb）逐渐减少,n（Alc）先增后减;随着OH/（Al+Mg+Ti）的增大,n（Ala）逐渐减少,n（Alb）、n（Alc）逐渐增加.③通过红外光谱、X-射线衍射,确定了PCAMT的结构组成,表明PCAMT是一种—OH桥联的铝镁钛复杂无定型聚合物,含有Al—OH—Mg与Ti—O—Ti新基团以及形成了Mg_1.5Ti_1.25O₄、Mg_1.2Ti_1.8O₅、Al₃Ti₅O₂等共聚物.④扫描电镜与能谱结果表明,PCAMT呈紧凑的空间立体网状形貌结构,利于发挥吸附架桥、网捕卷扫作用.⑤由PCAMT投加量对Zeta电位的影响分析可知,低投药量的混凝过程中起主导作用的是电中和作用,高投药量PCAMT处理原水的混凝机制以吸附架桥和网捕卷扫作用为主.研究显示,AlCl₃、MgCl₂和TiCl₄通过共聚反应,可生成具有更高聚合度的无定型共聚物PCAMT,利于电中和、吸附架桥和网捕卷扫,具有较好的混凝效果.      

还原增溶强化EGTA淋洗修复重金属污染土壤

采用还原剂调控土壤中重金属的活性,旨在强化其对乙二醇双(2-氨基乙基醚)四乙酸(EGTA)洗脱土壤重金属的洗脱效果.分析了EGTA投加量、还原剂类型、液固比、淋洗时间等对土壤重金属的影响,以及不同淋洗条件下土壤重金属浸出浓度与化学形态的差异,采用SEM-EDS和FTIR对处理前后土壤样品进行表征.结果表明,硫代硫酸钠(Na_2S_2O_3)可显著提高EGTA对重金属的洗脱率,当液固比为7.5∶1、淋洗时间为2 h、EGTA与Na_2S_2O_3投加量均为5 g·L~(-1)时,Cu、Zn、Pb和Cd洗脱率分别达85.0%、 60.7%、 88.6%和66.4%.与EGTA单独处理相比,EGTA/Na_2S_2O_3联合处理后, 4种重金属的浸出浓度均降低,Pb的降幅最大,土壤颗粒变小,团粒结构被破坏,O和Al含量减少,Si含量增加,降低了土壤矿物组分的吸附性;土壤有机质含量大幅降低,—OH振动显著减弱,配位能力较强的有机官能团减少,降低了土壤有机组分的吸附性.土壤中吸附性较强组分含量的降低是Na_2S_2O_3强化EGTA洗脱重金属的重要机制.     

Activated carbon coated palygorskite as adsorbent by activation and its adsorption for methylene blue

An activation process for developing the surface and porous structure of palygorskite/carbon(PG/C) nanocomposite using ZnC l2 as activating agent was investigated. The obtained activated PG/C was characterized by X-ray diffraction(XRD), Fourier transform infrared spectroscopy(FTIR), field-emission scanning electron microscopy(SEM), and Brunauer–Emmett–Teller analysis(BET) techniques. The effects of activation conditions were examined,including activation temperature and impregnation ratio. With increased temperature and impregnation ratio, the collapse of the palygorskite crystal structure was found to accelerate and the carbon coated on the surface underwent further carbonization. XRD and SEM data confirmed that the palygorskite structure was destroyed and the carbon structure was developed during activation. The presence of the characteristic absorption peaks of C_C and C–H vibrations in the FTIR spectra suggested the occurrence of aromatization. The BET surface area improved by more than 11-fold(1201 m2/g for activated PG/C vs. 106 m2/g for PG/C) after activation, and the material appeared to be mainly microporous. The maximum adsorption capacity of methylene blue onto the activated PG/C reached 351 mg/g. The activated PG/C demonstrated better compressive strength than activated carbon without palygorskite clay.     

Synergistic effect of N- and F-codoping on the structure and photocatalytic performance of TiO2

Three types of TiO₂ nanostructures were synthesized via a facile hydrolysis method at 195 °C. Effects of the preparation method and doping with N and F on the crystal structure and photocatalytic performance of TiO₂ were investigated. The nanomaterials were characterized by X-ray diffraction, transmission electron microscopy, X-ray photoelectron spectroscopy, Brunauer–Emmett–Teller porosimetry, ultraviolet–visible diffuse reflectance spectroscopy and fluorescent emission spectra. Their photo-catalytic activity was examined by the photodegradation of methylene blue in aqueous solution under both ultra-violet and visible light irradiation. The results show that nitrogen and fluorine co-doped anatase TiO₂ had the characteristics of a smaller crystalline size, broader light absorption spectrum and lower charge recombination than pure TiO₂. Most importantly, more efficient photocatalytic activity under both ultra-violet and visible light was observed. The obtained N–F-TiO₂ nanomaterial shows considerable potential for water treatment under sunlight irradiation.     

Comparison study of phosphorus adsorption on different waste solids: Fly ash, red mud and ferric–alum water treatment residues

The adsorption of phosphorus(P) onto three industrial solid wastes(fly ash, red mud and ferric–alum water treatment residual(FAR)) and their modified materials was studied systematically via batch experiments. Compared with two natural adsorbents(zeolite and diatomite), three solid wastes possessed a higher adsorption capacity for P because of the higher Fe, Al and Ca contents. After modification(i.e., the fly ash and red mud modified by FeCl_3 and FARs modified by HCl), the adsorption capacity increased, especially for the modified red mud, where more Fe bonded P was observed. The P adsorption kinetics can be satisfactorily fitted using the pseudo-second-order model. The Langmuir model can describe well the P adsorption on all of the samples in our study. p H and dissolved organic matter(DOM) are two important factors for P adsorption. Under neutral conditions, the maximum adsorption amount on the modified materials was observed. With the deviation from pH 7, the adsorption amount decreased, which resulted from the change of P species in water and surface charges of the adsorbents. The DOM in water can promote P adsorption, which may be due to the promotion effects of humic-Fe(Al) complexes and the pH buffer function exceeds the depression of competitive adsorption.     

Mg/Al LDH对UO22+的高效吸附研究

由于放射性污染物的不合理处置及核泄漏事件的发生,对生态环境和人类健康造成了严重危害.本研究采用共沉淀法制备了不同Mg/Al比(物质的量比)的Mg/Al LDH(层状双氢氧化物),研究其对UO_2~(2+)的吸附行为.同时,考察了吸附剂投加量、p H、吸附时间、初始浓度对吸附的影响,并采用XRD、FTIR、SEM、XPS等技术对吸附前后LDH材料进行表征与分析.结果表明:Mg/Al比为2∶1的Mg/Al LDH对UO_2~(2+)吸附效果要比Mg/Al比为4∶1的Mg/Al LDH好,Mg/Al比为2∶1和4∶1的Mg/Al LDH对UO_2~(2+)吸附容量分别为301.28和263.85 mg·g-1,对UO_2~(2+)具有优良的吸附性能,可以作为高浓度放射性污染废水的吸附材料和核泄漏事件的应急吸附材料.Mg/Al LDH对UO_2~(2+)的吸附更符合Langmuir等温吸附模型和Pseudo-second-order动力学模型.吸附后Mg/Al LDH的Mg/Al比降低,Mg/Al LDH对UO_2~(2+)的吸附机理是UO_2~(2+)与材料中氢氧根、碳酸根相互作用,形成三元的络合物而被去除.     

不同铁矿物对水稻土砷的稳定化效果及机制

水淹缺氧条件是驱动水稻土砷释放引起砷污染的主要原因,其中,铁矿物在砷的迁移转化过程中扮演重要的角色.为研究水铁矿、针铁矿和赤铁矿对水稻土砷的稳定化效果,分析了3种铁矿物对土壤溶液砷浓度的影响,采用土壤溶液中亚铁和总铁的浓度变化来评估不同铁矿物对砷的稳定化效果,并对3种铁矿物进行扫描电镜(SEM)和X射线衍射(XRD)等表征分析.结果表明,水铁矿具有最大的比表面积,为192.54m2·g-1,且微孔孔容达到0.069 cm3·g~(-1),针铁矿和赤铁矿依次减少,而3种铁矿物的结晶度以针铁矿最高,赤铁矿和水铁矿依次降低.施用水铁矿、针铁矿和赤铁矿均有效地降低了土壤溶液中砷的浓度,当添加量为2.0%(质量分数)时,土壤溶液中砷浓度分别降低62.55%、61.36%和55.16%.相关性分析表明,随着无定形铁含量的提高,其对砷的稳定化效果趋于显著,其中,土壤无定型铁与无定型结合态砷含量存在正相关关系(r=0.879,p=0.009),而与土壤溶液砷存在负相关关系(r=-0.895,p=0.006).     

蒙脱土、高岭土和针铁矿对DNA吸附与解吸特征

采用平衡法研究了蒙脱土、高岭土和针铁矿在不同pH值和不同电解质溶液下的DNA吸附解吸特征.结果表明,在4种电解质体系中,尤其在溶液pH值>5.0时,3种矿物在吸附过DNA后,pH有不同程度上升,但CaCl2电解质体系中含针铁矿溶液的pH开始下降.针铁矿对DNA的吸附率大约为75%～91%,高岭土对DNA的吸附率从pH为3.5时的90%开始下降,至pH 6.0～7.0时的下降至大约18%～50%.在一价电解质体系,当溶液pH值为2.2～5.0时蒙脱土对DNA的吸附率大约为90%开始下降至25%～40%,但在二价电解质体系蒙脱土对DNA的吸附率大约为92%.Freundlich等温吸附方程能更好的拟合针铁矿、蒙脱土和高岭土对DNA的吸附.蒙脱土对DNA相对吸附容量在pH 3.5时大于针铁矿,而pH 5.0时小于针铁矿.以NaOAc为解吸剂,针铁矿、蒙脱土和高岭土上吸附DNA在不同pH时解吸率分别为0.1%～0.4%、63.7%～90.2%和29.7%～87.5%.以NaH2PO4为解吸剂时,这些矿物吸附DNA的解吸率分别为69.6%～78.7%、0.8%～7.0%和0.4%～2.2%.这表明针铁矿吸附DNA时键合作用较大,蒙脱土和高岭土静电引力较大,这是DNA在不同电荷类型矿物表面的吸附差异.     

Insight into the adsorption of tetracycline onto amino and amino–Fe functionalized mesoporous silica: Effect of functionalized groups

In order to study the influences of functionalized groups onto the adsorption of tetracycline (TC), we prepared a series of amino and amino–Fe^3 + complex mesoporous silica adsorbents with diverse content of amino and Fe^3 + groups (named N,N-SBA15 and Fe-N,N-SBA15). The resulting mesoporous silica adsorbents were fully characterized by X-ray powder diffraction, Fourier transform infrared spectrometer and N₂ adsorption/desorption isotherms. Furthermore, the effects of functionalized groups on the removal of TC were investigated. The results showed that the periodic ordered structure of SBA-15 was maintained after modification of amino/Fe^3 + groups. The functionalized amino groups decreased the adsorption capacity while the coordinated Fe^3 + increased the adsorption capacity. The adsorption kinetics of TC fitted pseudo-second-order model well and the equilibrium was achieved quickly. The adsorption isotherms fitted the Langmuir model well and with the Fe^3 + content increased from 3.93% to 8.26%, the Q_max of the adsorbents increased from 102 to 188 mmol/kg. The solution pH affected the adsorption of TC onto amino complex adsorbents slightly while influenced the adsorption onto Fe-amine complex adsorbents greatly. The adsorption of TC on SBA15 and N,N-SBA15 may be related to the formation of outer-sphere surface complexes, while the adsorption of TC onto Fe-N,N-SBA15 was mainly attributed to the inner-sphere surface complexes. This study could offer potential materials that have excellent adsorption behavior for environmental remediation and suggested useful information for the preparing other adsorbents in environmental applications.     

Removal of arsenate with hydrous ferric oxide coprecipitation：Effect of humic acid

Insights from the adverse effect of humic acid(HA) on arsenate removal with hydrous ferric oxide(HFO) coprecipitation can further our understanding of the fate of As(V) in water treatment process. The motivation of our study is to explore the competitive adsorption mechanisms of humic acid and As(V) on HFO on the molecular scale. Multiple complementary techniques were used including macroscopic adsorption experiments, surface enhanced Raman scattering(SERS), extended X-ray absorption fine structure(EXAFS) spectroscopy, flow-cell attenuated total reflectance Fourier transform infrared(ATR-FTIR) measurement, and charge distribution multisite complexation(CDMUSIC) modeling. The As(V) removal efficiency was reduced from over 95% to about 10% with the increasing HA concentration to 25 times of As(V) mass concentration. The SERS analysis excluded the HA-As(V) complex formation. The EXAFS results indicate that As(V) formed bidentate binuclear surface complexes in the presence of HA as evidenced by an As-Fe distance of 3.26–3.31 ?. The in situ ATR-FTIR measurements show that As(V) replaces surface hydroxyl groups and forms innersphere complex. High concentrations of HA may physically block the surface sites and inhibit the As(V) access. The adsorption of As(V) and HA decreased the point of zero charge of HFO from 7.8 to 5.8 and 6.3, respectively. The CD-MUSIC model described the zeta potential curves and adsorption edges of As(V) and HA reasonably well.