棉花模板Zn/Ti/Fe-LDO吸附水中硝酸盐机制

通过共沉淀-焙烧法制备以棉花为模板的Zn/Ti/Fe焙烧态类水滑石(YLDO)和无棉花模板的Zn/Ti/Fe焙烧态类水滑石(NLDO),运用SEM、N2吸附法、FTIR和XRD对其进行表征,考察YLDO和NLDO对水中硝酸盐的吸附机制及其紫外光催化再生的机理。结果表明,YLDO在形态中引入棉花的遗迹,比表面积增大为74.8 m2·g-1,大孔数量增加;在化学成分上引入了C元素,提高了吸附性能;形成磁性物质,可通过磁性分离回收。pH为7、298K时,YLDO对水中硝酸盐的最大吸附量为66.57mg·g-1,比NLDO增加了22.6%。YLDO和NLDO吸附硝酸盐的吸附等温线符合Langmuir方程,吸附动力学可用准二级动力学方程来描述,吸附热力学研究表明吸附过程为自发吸热过程。吸附饱和的YLDO和NLDO可在紫外光照射下再生,5次再生循环后仍保持较高的吸附性能。YLDO可通过吸附-磁分离-紫外光催化再生工艺有效去除水中硝酸盐,不产生二次污染,在硝酸盐废水处理中具有潜在的应用前景。     

酸性黄17在焙烧态Zn/Al水滑石上的吸附研究

研究了摩尔比为3:1的焙烧态水滑石(Zn/Al-LDO)对酸性黄17(AY17)的吸附。考察了AY17不同起始浓度C0、温度及p H值等因素对Zn/Al-LDO吸附AY17的影响,并探讨了吸附过程的动力学和热力学规律。实验结果表明:Zn/Al-LDO对AY17具有良好的去除效果,在25℃、p H=7条件下,0.5 g?L?1的Zn/Al-LDO对C0=50~200 mg?L?1的AY17去除率超过98%。动力学和热力学研究表明:Zn/Al-LDO对AY17的吸附过程均符合Langmuir和Freundlich等温吸附方程,且是一个自发、放热的过程。由D–R等温吸附方程计算的吸附自由能E为0.1474~1.6667 k J?mol?1,表明吸附过程为物理吸附。同时,该吸附过程符合准二级反应动力学模型。通过XRD、FT-IR及颗粒内扩散模型的实验数据进一步分析吸附机理,推断膜扩散和颗粒内扩散对Zn/Al-LDO吸附AY17起决定性作用。     

吸附法脱除水中硫酸根技术进展

硫酸根是无机化工行业、工业废水、矿井废水、地表水以及饮用水中常见的阴离子，它的大量存在给化工生产、环境和人类健康造成不利影响，因此，探索出脱除水中硫酸根的有效、经济的方法具有重要的现实意义。目前，脱除水中硫酸根的方法很多，主要综述了水中硫酸根的吸附脱除法，包括NDS法、石灰和聚合氯化铝结合法、焙烧水滑石吸附法、柱撑蒙脱石吸附法、针铁矿吸附法、氢氧化铁吸附法、离子交换法，并指出了各种方法的原理和特点。同时展望了今后的研究发展方向。     

Mg/Al双金属氧化物吸附Cr(Ⅵ)的动力学和热力学机理

通过静态吸附实验,研究了Cr(Ⅵ).Mg/Al水滑石焙烧产物层状双金属氧化物(layered double oxides,LDO)的吸附性能.考察了温度对其吸 附性能的影响,探讨了吸附动力学和热力学规律.研究表明:吸附动力学符合准二级动力学模型,LDO的吸附活化能为21.42kJ/mol,表现为扩散控 制过程.在293~333 K温度范围内,吸附自由能(△Go)变小是Cr(Ⅵ)ELDO上的吸附推动力;吸附热(吸附焓变H)为5.12 kJ/mol,是自发的物理吸附过程;LDO吸附Cr(Ⅵ)为熵增过程.其熵变为49.12 J/(mol·K).结合XRD表征结果探讨了吸附机理:LDO吸附Cr(Ⅵ)无配位摹交换、化学键等强的作用力,Mg/Al金属氧化物在吸附Cr(Ⅵ)后恢复为LDH层状结构,因此,LDO对Cr(Ⅵ)的强吸附能力是冈为其具有较强的结构"记忆效应".     

水滑石及其焙烧产物对水中苯甲酸根的吸附研究

为了脱除水中的苯甲酸根,以苯甲酸作为吸附质,研究了水滑石及其焙烧产物的吸附作用。考察了吸附剂的镁铝摩尔比、初始pH值、苯甲酸浓度、吸附剂添加量、吸附时间和温度对吸附效果的影响,并对比考察水滑石和焙烧水滑石对苯甲酸的吸附。结果表明,水滑石及其焙烧产物对苯甲酸的最优吸附条件均为酸性环境下,镁铝摩尔比3∶1,吸附质浓度220 mg/L,吸附剂的量0.06 g;水滑石吸附时间20 h,吸附温度为60℃时,对苯甲酸的去除效果最好;而焙烧水滑石在室温下吸附苯甲酸8 h达到最高去除率;在同样条件下,水滑石焙烧产物比水滑石对苯甲酸的吸附大得多。     

Zn/Cr水滑石吸附-可见光催化水中有机污染物

通过共沉淀法合成可循环使用的阴离子粘土材料锌铬水滑石(Zn/Cr LDHs),并借助X射线衍射(XRD),N2吸附-脱附曲线,扫描电子显微镜(SEM)和紫外-可见光漫反射光谱(DRS)等对其进行表征分析。以刚果红为模型污染物,研究了Zn/Cr LDHs去除有机污染物的吸附-可见光光催化活性。通过等温吸附试验,得到Langmuir等温线,其饱和吸附量为426.29 mg/g。Zn/Cr LDHs在氙灯模拟太阳光照射下,每次试验180 min,第5次后脱色率仍高达96.35%,具有良好的可循环使用性。刚果红吸附等温线符合Langmuir模型,吸附过程符合拟二级动力学模型,内扩散为主要控速步骤,吸附过程是自发的放热过程,低温有利于吸附的进行。     

Zn/Al类水滑石对气态碘单质的吸附

用液相非稳态共沉淀法合成了Zn/Al类水滑石(Zn/Al-HTLcs)。Zn/Al-HTLcs能吸附气态碘单质,且被碘离子饱和的Zn/Al-HTLcs能快速吸附气态碘单质。吸附温度和Zn/Al-HTLcs中碘离子的含量明显影响碘单质的吸附速率与吸附量。通过X射线晶体粉末衍射(XRD)研究了Zn/Al-HTLcs和碘离子饱和Zn/Al-HTLcs吸附气态碘单质样品(In-+Zn/Al-HTLcs)的结构特征,证实吸附碘后,层板结构没有改变而层间距略有增大。In-+Zn/Al-HTLcs在高于碘单质沸点的温度下,仍具有良好的热稳定性,其中碘的存在形态为碘多阴离子。     

去除水中腐殖酸的磁性焙烧态类水滑石制备与表征

采用共沉淀法一步合成系列类水滑石负载磁性粒子的颗粒,经煅烧得到磁性焙烧产物.利用焙烧产物吸附水中腐殖酸,得到磁性焙烧态锌铝类水滑石去除腐殖酸效果较好.考察了磁性焙烧态锌铝类水滑石制备条件对腐殖酸去除效果的影响,通过正交试验优化了制备条件.静态吸附实验表明:吸附剂投加量0.2 g/L, 30 min内20 mg/L腐殖酸去除率为97.96%.X射线衍射(XRD)、红外光谱(FT-IR)、热重-差热(TG-DSC)和比表面积(SSA)表征结果表明:一定量的磁性基质掺入并没有破坏锌铝类水滑石典型的层状结构;焙烧态产物为氧化物,磁性保持良好;比表面积达80.00 m2/g.磁性焙烧态锌铝类水滑石在水中因"记忆效应"而结构重建通过表面吸附和腐殖酸结构中小尺寸的官能团插层快速去除腐殖酸.     

磁性类水滑石的制备和吸附水中磷的研究

采用共沉淀制备一系列磁性Mg-Al、Zn-Al、Mg-Fe和Zn-Fe类水滑石磷吸附剂,并研究了磁性类水滑石的组成、摩尔比、pH值、吸附剂用量等对含磷酸盐废水的吸附性能影响。结果表明,磁性类水滑石对磷酸根有良好的吸附效果,磁性类水滑石的金属组成对磷酸根吸附有显著影响,其中Mg/Al摩尔比为2∶1的磁性类水滑石在pH=5～7范围内吸附效果最好,吸附剂最佳投加量0.5 g,最高吸附量达47.1 mg/g。     

镁铝二元水滑石焙烧产物对酸性紫90染料的吸附性能(英文)

研究了镁铝比为3:1的二元水滑石(layered double hydroxides)焙烧产物(MgAl–LDO,layered double oxide)对弱酸性染料酸性紫90(C40H27CrN8Na2O10S2,AV90)的吸附性能。X射线衍射和Fourier变换红外光谱的结果显示:由于水滑石的"结构记忆效应",在富水条件下,MgAl–LDO会吸附部分AV90阴离子进入水滑石层间,从而恢复为层状结构的MgAl–LDHs。研究结果表明:MgAl–LDO对AV90具有良好的去除效果,在298 K,pH=9.7条件下,MgAl–LDO对AV90去除率高达99.7%,吸附容量为999.78 mg/g。MgAl–LDO对AV90的吸附过程同时符合Langmuir和Freundlich等温吸附方程,并且是一个自发、放热的过程。动力学研究表明:该吸附动力学符合准二级动力学模型。吸附实验结果同时表明:MgAl–LDO吸附性能优于活性炭和二氧化硅等传统吸附剂,经三次回收利用的MgAl–LDO对AV90仍具有良好的吸附性能。     

可光助再生二氧化钛/层状双氢氧化物去除水体中有机染料

利用吸附-光催化技术去除水体中有机染料,是高效节能的方法之一。然而,碳基吸附剂在光催化降解污染物过程中,由于活性氧的攻击会发生自身的逐渐氧化。本研究中,采用尿素水解水热法制备二氧化钛/层状双氢氧化物(TiO₂/LDH)非碳基复合材料,不仅对水体中有机染料具有较高的吸附容量,也在光辐射后具有可重复的再生能力。对甲基橙的吸附量为527.5 mg/g,在4轮循环再生后仍具有88.6%的再生率;对亚甲基蓝的吸附量为208.3 mg/g,在4轮循环再生后仍具有94.7%的再生率。在吸附-光再生过程中,LDH基底自身具有强抗氧化能力和高吸附能力,同时提高了负载剂TiO₂的光吸收效率,为水中有机污染物去除和吸附-光催化复合材料设计优化提供了可行的策略。     

层状双金属氢氧化物吸附剂的功能化改性策略

层状双金属氢氧化物（LDHs）是一类阴离子交换能力强、可调性好、热稳定性高、活性位点丰富的纳米吸附材料,在水中污染物的吸附去除方面呈现出巨大潜力。然而,官能团和结构组分的缺陷严重限制了原始LDHs的吸附性能和应用范围。利用不同改性策略对LDHs进行功能化处理,能显著增强LDHs的污染物吸附容量、选择性、稳定性、可回收性以及适用范围。该文从LDHs吸附水中污染物性能的优化出发,重点综述了当前常用的插层、表面修饰、煅烧、复合组装、包埋、制膜等LDHs功能化改性策略,总结了其与水中各种污染物（无机非金属阴离子、重金属离子、染料以及抗生素）之间的作用机理。此外,还阐述了相应的再生手段。最后,简要提出了功能化LDHs吸附剂的优势以及后期研究可能面临的障碍,并对其广阔的应用前景进行了展望。     

Adsorption of reactive dyes from aqueous solutions by layered double hydroxides

BACKGROUND: Water‐soluble reactive azo dyes are the most problematic dye house effluents, as they tend to pass through conventional treatment systems unaffected. The release of these compounds into the environment is undesirable and their removal becomes environmentally important. In this work, synthesis, characterization and sorption properties of hydotalcite‐like compounds (Mg/Al and Mg/Fe), calcined and uncalcined, were investigated for the removal of the reactive azo dye Remazol Red 3BS. RESULTS: The calcined compounds present higher surface area than the uncalcined. The optimum pH for sorption was found to be 6. Thermodynamic analysis reveals that the sorption is spontaneous and endothermic. Equilibrium data were fitted by a Langmuir model, and kinetic data by a second‐order model. The calcined Mg/Al compound showed the highest sorption capacity, at 0.125 mmol g^?1. Regeneration of dye loaded derivative is achieved using the surfactant SDS. CONCLUSIONS: The prepared hydotalcite‐like compounds and especially calcined Mg‐Al exhibited significant adsorption capacity, kinetics, and regenerative ability. Its potential applicability as sorbent should be tested in a large‐scale implementation. Copyright © 2011 Society of Chemical Industry     

Adsorption of phosphate by layered double hydroxides in aqueous solutions

Adsorption of phosphate by various calcined layered double hydroxides (LDHs) such as Mg–Al, Zn–Al, Ni–Al, Co–Al, Mg–Fe, Zn–Fe, Ni–Fe and Co–Fe was investigated. LDHs were found to have high anion exchange capacity that enhances their capability to remove anionic contaminants from aqueous system. The nature and content of di- and trivalent cations in LDH have strong influence on the adsorption process. Calcined Mg–Al LDH (CLDH) with Mg–Al molar ratio of 2.0 showed higher adsorption capacity compared to other calcined LDHs as it possessed higher Al³⁺ content. Results indicate that the adsorption isotherm could be fitted to a linearised form of Langmuir and Freundlich equations. The adsorption phenomenon has been well supported by XRD study. The adsorption process was spontaneous and exothermic in nature and followed first order kinetics. Competitive anions were found to have detrimental effect on the percentage of adsorption.     

层状双氢氧化物材料在染料废水中的应用进展

层状双氢氧化物(LDH)凭借其特殊的层状结构、极强的可调控性等,已在水处理领域得到广泛关注.LDH除用于重金属吸附外,处理染料废水也表现出独特的优势.但由于单一的LDH存在耐酸碱性差、表面官能团少、化学稳定性差等缺陷,严重制约了其在处理染料废水方面的应用,为此,越来越多的研究者通过对LDH进行改性提高材料的吸附性能.首先归纳总结了LDH材料的常用制备及改性方法并比较了各方法的优缺点;其次,介绍了改性LDH材料对染料废水中离子的去除效果及其吸附机理,同时分析了不同环境条件(pH、接触时间、吸附剂用量等)对LDH基吸附材料吸附性能的影响;最后,对改性LDH材料的应用现状作出总结并对其未来发展方向作出展望.     

Ce cooperated layered double oxide with enhanced base sites activity for the synthesis of polycarbonate diols

The development of highly efficient alkaline catalysts with abundant base sites is of paramount importance for the synthesis of polycarbonate diols (PCDLs). And the application of heterogeneous catalysts is an effective strategy to address the effect of residual catalysts on the quality of PCDLs. Here, Ce cooperated layered double oxide (LDO-Ce) was used as a catalyst for the preparation of PCDLs via transesterification between dimethyl carbonate (DMC) and 1,4-butanediol (BDO). CO₂ temperature-programmed desorption (CO₂-TPD) profiles demonstrated that the introduction of Ce led to an increase in strong base sites of LDO-Ce, thus endowing LDO-Ce with excellent catalytic performance. Besides, LDO-Ce possessed satisfactory specific surface area and pore size. A possible catalytic mechanism was proposed to illustrate the transesterification process. The effects of the reaction conditions on the hydroxyl value, yield, and BDO conversion were further investigated in detail. The yield of PCDLs with a hydroxyl value of 112.2 mg KOH/g (corresponding to a number average molecular weight [M_n] of 1000 g/mol) was 92.44% under its optimum reaction conditions (w (catalyst) = 0.5%, n(DMC)/n(BDO) = 1.25, T-_{transesterification} = 130°C, t-_{transesterification} = 5 h, T-_{polycondensation} = 170°C, t-_{polycondensation} = 4 h, P-_{polycondensation} = 10 kPa). Moreover, LDO-Ce was easily removed after the transesterification process (Step 1), ensuring the quality of PCDLs, and it was recycled three times without significant loss of catalytic activity.     

氧化铁/层状双金属氢氧化物复合材料的制备

制备由不同结构单元组成的复合材料是提高材料性能的一种有效方法.分别采用两种方式(双滴共沉淀法和LDHs层板附着生长法)制备Fe3 O4/层状双金属氢氧化物(LDHs)复合材料.利用X-射线衍射、电子显微分析和红外光谱等测试方法研究了LDHs和Fe3 O4的复合方式对复合材料形貌、粒径和结晶性能的影响.同时对比分析了两种制备方案得到的Fe3OJLDHs复合材料生长规律.实验结果表明,采用双滴共沉淀法制备的Fe3OJLDHs复合材料具有层状结构和良好的结晶性.     

锌铝水滑石微米球的合成及吸附性能研究

采用多步法合成锌铝复合氧化物（LDO）与锌铝水滑石（LDHs）,通过XRD、SEM、TEM、N2吸附等对合成的试样进行了表征;研究了甲基橙（MO）在LDO及LDHs上的吸附性能,考察了pH值和温度对吸附性能的影响,并结合红外光谱和XRD对吸附机理进行探讨.结果表明：所制备的LDO和LDHs呈空心球状,直径为3～5 μm,分散性较好,LDO比表面积高达210.2 m2/g;LDO对甲基橙具有优异的吸附性能,在25℃,初始pH=3的条件下,0.2 g/L LDO对100 mg/L甲基橙的吸附容量和去除率分别达497 mg/g和99.4％,其吸附等温线和吸附动力学分别符合Langmuir方程和准二级速率方程.     

Co/Fe类水滑石活化过硫酸盐降解苯酚特性

采用共沉淀法制备了Co/Fe类水滑石（Co/Fe-LDHs）,焙烧后得到了焙烧态Co/Fe类水滑石（Co/Fe-LDO）,通过XRD、SEM、BET、XPS等手段对样品的晶体结构及表面形貌进行了表征,考察了其活化过硫酸盐降解苯酚的影响因素及机理。结果表明,焙烧可使类水滑石比表面积从41.2 m2/g增大至56.8 m2/g,孔体积从0.2 cm3/g增大至0.3 cm3/g,增强了对过硫酸盐的活化性能。在反应时间30.0 min,反应温度25.0℃,过硫酸钠投加量为0.2 g/L,Co/Fe-LDO投加量为0.2 g/L,pH为6.0,初始苯酚浓度为100.0 mg/L时,苯酚降解率可达90.1%。 Co/Fe-LDO活化过硫酸钠降解苯酚反应过程中SO4−•和•OH起主要作用。     

Synergistic effect of V and Fe in Ni/Fe/V ternary layered double hydroxides for efficient and durable oxygen evolution reaction

High-performance and stable electrocatalysts are vital for the oxygen evolution reaction (OER). Herein, via a one-pot hydrothermal method, Ni/Fe/V ternary layered double hydroxides (NiFeV-LDH) derived from Ni foam are fabricated to work as highly active and durable electrocatalysts for OER. By changing the feeding ratio of Fe and V salts, the prepared ternary hydroxides were optimized. At an Fe:V ratio of 0.5:0.5, NiFeV-LDH exhibits outstanding OER activity superior to that of the binary hydroxides, requiring overpotentials of 269 and 274 mV at 50 mA·cm^–2 in the linear sweep voltammetry and sampled current voltammetry measurements, respectively. Importantly, NiFeV-LDH shows extraordinary long-term stability (≥ 75 h) at an extremely high current density of 200 mA·cm^–2. In contrast, the binary hydroxides present quick decay at 200 mA·cm^–2 or even reduced current densities (150 and 100 mA·cm^–2). The outstanding OER performance of NiFeV-LDH benefits from the synergistic effect of V and Fe while doping the third metal into bimetallic hydroxide layers: (a) Fe plays a crucial role as the active site; (b) electron-withdrawing V stabilizes the high valence state of Fe, thus accelerating the OER process; (c) V further offers great stabilization for the formed intermediate of FeOOH, thus achieving superior durability.