氧化程度对氧化石墨烯吸附亚甲基蓝性能的影响

基于改进Hummers法,调控氧化剂KMnO_4用量制备了不同含氧官能团含量的氧化石墨烯(GOs)。采用XRD、XPS、AFM和FTIR分析了KMnO_4用量对GOs的结构特征、含氧官能团类型及含量的影响,研究了氧化程度对GOs吸附亚甲基蓝(MB)性能的影响。结果表明:KMnO_4用量对GOs-n(n=2,3,4)的含氧官能团类型和含量有显著影响;MB最大饱和吸附量依次为728.44、965.63和807.29 mg·g~(-1),与Langmuir模型单分子层饱和吸附量的标准差为3.6%、3.7%和4.2%,吸附动力学过程符合准二级动力学模型,R~20.99。以GOs结构层上去质子化的羟基(—C—O~-)和羧基(—COO~-)为主要活性位点与MB发生化学控速的单分子层放热吸附,吸附热在20~27 kJ·mol~(-1)之间;低氧化程度的GOs以离子交换吸附为主导,吸附性能与GOs结构中—C—O(H)和—COO(H)的总量呈正相关。随氧化程度加深,GOs结构中环氧基(C—O—C)和羰基(C═O)以氢键作用吸附MB对吸附量的影响凸显。     

TEPA负载复合氧化活性炭吸附烟气中的CO2性能

以商业煤基活性炭为原料，经低浓度氧气焙烧、H₂O₂氧化改性，并以四乙烯五胺（TEPA）浸渍，得到胺负载复合氧化活性炭，用于模拟烟道气[(15%(体积)CO₂+85%(体积)N₂）+10%(体积)H₂O]中CO₂吸附。低浓度氧气焙烧后，活性炭的最大比表面积和孔体积分别为1421.82 m²/g、0.83 cm³/g。经复合氧化改性后，活性炭的介孔体积增大，表面含氧官能团增加，使得TEPA负载复合氧化活性炭的CO₂吸附性能提高。焙烧时间为4 h，H₂O₂氧化、负载40%TEPA的样品COAC-4-40TEPA，在60℃时CO₂饱和吸附量最高为2.45 mmol/g，是TEPA负载未改性活性炭AC-40TEPA的2.02倍。经过十次吸附循环后，COAC-4-40TEPA的 CO₂饱和吸附量可维持在92.24%，而TEPA的浸出量仅有0.67%。失活模型研究表明，COAC-4-40TEPA的初始吸附速率常数是AC-40TEPA的1.64倍，且失活速率常数低于AC-40TEPA。     

乳液法制备石墨烯气凝胶及其吸附水中亚甲基蓝

利用乳液法制备多孔石墨烯气凝胶（emGA）,改变乳液油水比制备不同的emGA。扫描电子显微镜（SEM）、傅里叶红外光谱（FTIR）、氮气吸附脱附等表征显示,emGA具有多孔结构,经水热还原后含氧官能团大部分被除去,比表面积为103.3～243.1m²/g。以亚甲基蓝（MB）浓度和温度作为变量,考察emGA对水中MB的吸附效果。结果表明,emGA的比表面积越大,其对MB平衡吸附量越大;当初始浓度越大,温度越高,则吸附有利。吸附动力学数据表明emGA吸附MB符合准二级动力学模型和内扩散模型,吸附过程分为大孔扩散和微孔扩散。吸附等温线数据拟合结果符合Langmuir模型,表明emGA对MB的吸附属于单分子层吸附。Langmuir模型计算出emGA-2饱和吸附量为307.7mg/g,与实验值291.3mg/g较为接近。分析热力学参数发现,emGA吸附MB为自发吸热过程,且吸附过程属于物理吸附。     

不同氧化程度氧化石墨烯氨气敏感性能及机理

基于改进的Hummers法,通过改变氧化剂KMnO_4用量制备了各种含氧官能团含量差异明显的氧化石墨烯(GOs)水相分散液,采用旋涂法制备了厚度均一的GOs气敏元件。利用XRD、FTIR、XPS对样品的结构、官能团种类及含量进行了分析;利用气敏测试系统对GOs气敏元件的NH_3敏感性能进行了测试。结果表明:GOs含有羟基(—OH)、环氧基〔—CH(O)CH—〕等含氧官能团,随KMnO4用量的增加,GOs中羟基(—OH)的相对含量(XPS测得)先增加后减少,当m(KMnO_4)∶m(石墨)=3∶1时,—OH的相对含量最高。不同氧化程度的GOs气敏元件对NH_3灵敏度与其—OH的相对含量呈正相关性,GOs中—OH相对含量为43.75%时,气敏元件对体积分数为0.008%的NH_3最大灵敏度达到78%,且有较好的稳定性和重复性,重复性误差为3.1%。GOs对NH_3分子的响应存在两种机制:NH_3分子进入GOs片层间水分子层后水解形成NH_4~+的离子电导,和GOs结构层上含氧官能团对NH_3分子吸附后形成氢键的电荷转移。     

花生壳生物炭的改性及其吸附Pb2+性能研究

以花生壳为原料热解制备生物炭,并分别采用NaOH和KMnO₄进行改性,经表征发现改性后生物炭微观结构较为疏松、孔径变小、稳定性增强,NaOH改性花生壳生物炭（AB）和KMnO₄改性花生壳活性炭（MnB）的比表面积分别增至花生壳生物炭（B）的3.178倍和5.065倍,以KMnO₄作为改性剂时,锰氧化物成功地固定在生物炭上,B、AB和MnB的零电荷点（pH_PZC）分别为2.193、2.888和2.466。探究改性前后生物炭对Pb²⁺的吸附性能发现：B、AB和MnB吸附Pb²⁺的适宜pH值分别为4.5~6.5、5.5~6.5和5.0~6.5,达到相同Pb²⁺去除率时,生物炭用量MnB 2+的吸附平衡时间较B吸附Pb²⁺的吸附平衡时间（1 080 min）分别缩短了180和480 min。通过吸附动力学模型和等温线模型分析可知,3种生物炭吸附Pb²⁺的过程均受化学吸附控制,吸附速率MnB>AB>B,AB和MnB的最大理论吸附量分别是53.19和80.65 mg/g,分别提高至B的1.38倍和2.10倍。     

酸化高锰酸钾溶液处理的氯丁橡胶表面的粘合性能研究

采用硫酸酸化高锰酸钾(KMnO₄)溶液(H⁺/KMnO₄溶液)对氯丁橡胶(CR)(硫化胶)进行表面改性处理,研究KMnO₄质量分数、pH值和温度对CR表面的性质、化学组成、粗糙度以及CR表面与阻燃涂层的粘合性能的影响。结果表明：H⁺/KMnO₄溶液处理的CR表面粗糙且生成大量含氧基团,CR表面与阻燃涂层的粘合性能提高;H⁺/KMnO₄溶液对CR表面处理的最佳条件为KMnO₄质量分数5%,pH值1.44,温度60℃。     

向日葵制活性炭对亚甲基蓝的吸附研究

含有亚甲基蓝（MB）的废液直接排放会造成严重的水体污染。为研究生物质活性炭对MB的吸附性能,以农业废弃物向日葵为原料、磷酸（H₃PO₄）为活化剂,制备粉状活性炭（PAC）和块状活性炭（BAC）,并研究PAC对MB的吸附性能。利用比表面积测试（BET）、X射线光电子能谱（XPS）、X射线衍射（XRD）、红外光谱（FT-IR）和扫描电镜（SEM）等方法解析活性炭的孔结构和表面特性。结果表明：活性炭前驱体的形状对活性炭的微观结构有较大的影响。PAC比BAC具有更大的比表面积（分别为701.95 m²/g和566.49 m²/g）和总孔体积（分别为2.23 cm³/g和1.04 cm³/g）;PAC和BAC的平均孔径分别为7.31 nm和12.66 nm,均具有介孔材料的结构特性。两种活性炭表面均分布着丰富的含氧官能团和大量疏松的无定形碳,而存在的偏磷酸盐对孔隙起到支撑作用,这为MB的吸附提供了更多的活性位点和吸附通道。在25 ℃、pH为8、PAC用量为50 mg条件下,PAC对100 mL质量浓度为200 mg/L的MB溶液的吸附效果最好,吸附率达到72.2%。吸附过程符合伪二级动力学模型、颗粒内扩散模型和Langmuir等温吸附模型。     

交联淀粉负载氢氧化镁复合材料对Cu2+的吸附性能

以交联淀粉和MgSO₄·7H₂O为原料，NaOH为碱化剂，制备了交联淀粉负载氢氧化镁复合材料IStMg(OH)₂，采用FTIR、SEM、EDS、XRD对其进行了表征，并将其用于对模拟废水中Cu²⁺的吸附去除，考察了IStMg(OH)₂投加量、pH、Cu²⁺初始浓度等因素对ISt-Mg(OH)₂吸附Cu²⁺性能的影响。结果表明，当Cu²⁺质量浓度为20mg/L,pH=5.32,ISt-Mg(OH)₂投加量为300 mg/L，吸附温度为25 ℃时，Cu²⁺的去除率可达91.7%。吸附等温线拟合结果表明，ISt-Mg(OH)₂对水中Cu²⁺的吸附过程符合Langumir吸附模型，为单分子层吸附过程，在25 ℃时，拟合饱和吸附量为82.78 mg/g。吸附动力学数据拟合结果表明，吸附过程符合准二级动力学模型，属于...     

活性炭纤维氧化改性后的脱硫性能

为了将活性炭纤维（ACF）应用于空调领域实现新风的过滤优化以及提高吸附极性分子SO₂的效率,对ACF进行液相氧化改性制成了具有极性的折叠式复合体滤网,并进行了SEM、BET和FTIR分析;搭建了直流式系统实验台,选用甲醛吸收-副玫瑰苯胺分光光度法检测室外空气进入滤网前后SO₂的浓度,定量研究了在不同初始SO₂浓度下改性前后滤网的动态脱硫效率。结果表明：① ACF经HNO₃氧化改性处理后,表面微观结构有显著变化,比表面积、孔容、孔径分别由653.70m²/g、0.43cm³/g、2.64nm降低至488.84m²/g、0.32cm³/g、2.58nm,O—H和C—O的透射率分别由96%、95%降低至65.5%、75%,即表面酸性含氧官能团（羟基、羧基和醚基）含量增加;② 改性前后ACF对低浓度SO₂的平均动态脱硫效率分别为33%和75%,即改性后ACF的表面极性增强,滤网的动态脱硫效率提高了42%,应用于空调过滤网可有效改善室内空气品质。     

氧化石墨烯-TiO2复合材料对三种染料的吸附动力学及光催化性能

通过在氧化石墨烯分散溶液中水解钛酸丁酯成功制备氧化石墨烯-TiO₂复合材料（GO-TiO₂）,采用傅里叶变换红外光谱（FTIR）、X射线衍射（XRD）、扫描电子显微镜（SEM）、X射线光电子能谱（XPS）、全自动比表面及孔径分析仪（BET）和紫外-可见漫反射光谱（UV-vis DRS）等对样品进行了表征。研究了GO10-TiO₂对亚甲基蓝（MB）、甲基橙（MO）和罗丹明B（RhB）3种染料的吸附动力学和光催化性能。结果表明：TiO₂颗粒均匀地附着在GO片层表面;GO10-TiO₂对3种染料的吸附过程为多层吸附,吸附动力学符合拟二级动力学模型;在25℃条件下GO10-TiO₂对废水中MB、MO和Rh B的吸附因共轭结构、极性等的差异而呈现选择性吸附,吸附容量分别为9.2mg/g、5.4mg/g和23.0mg/g。对3种染料废水的光催化降解效果与吸附性能相关联,吸附容量越大降解效率越高,光催化反应60min时,MB、MO和Rh B降解率分别为89%、75%和98%。     

Adsorption equilibrium for Z-ligustilide on C18-bonded silica from supercritical carbon dioxide

Adsorption equilibrium is of great importance for the preparative supercritical fluid chromatography(pre-SFC) in defining supercritical adsorption behavior and the industrial amplification.This paper presents adsorption isotherms of Z-ligustilide from supercritical carbon dioxide(SC-CO_2) on C18-bonded silica.Adsorption behavior was studied at 305.15 K,313.15 K and 323.15 K with SC-CO_2 density varying from 0.687 g·cm~(-3) to0.863 g·cm~(-3) with the elution by characteristic points(ECP) method.The adsorption amount of Z-ligustilide from SC-CO_2 on C18-bonded silica decreased with the increasing density of the mobile phase as well as the increasing temperature.Adsorption equilibrium data were fitted by Langmuir and Freundlich isotherm models,and the Langmuir isotherm model performed better for describing the whole adsorption process on the column.The monolayer saturation adsorption capacity of Z-ligustilide is in the range of 3.0 × 10~(-4) mg·cm~(-3) to5.5 × 10~(-4) mg·cm~(-3) with an average value of 4.0 × 10~(-4) mg·cm~(-3).     

From pollutant to solution of wastewater pollution: Synthesis of activated carbon from textile sludge for dye adsorption

Adsorption is an important process in wastewater treatment,and conversion of waste materials to adsorbent offers a solution to high material cost related to the use of commercial activated carbon.This study investigated the adsorption behaviour of Reactive Black 5(RB5)and methylene blue(MB)onto activated carbon produced from textile sludge(TSAC).The activated carbon was synthesized through chemical activation of precursor followed with carbonization at 650°C under nitrogen flow.Effects of time(0–200 min),pH(2–10),temperature(25–60°C),initial dye concentration(0–200 mg·L~(-1)),and adsorbent dosage(0.01–0.15 g)on dye removal efficiency were investigated.Preliminary screening revealed that TSAC synthesized via H_2SO_4activation showed higher adsorption behaviour than TSAC activated by KCl and ZnCl_2.The adsorption capacity of TSAC was found to be 11.98 mg·g~(-1)(RB5)and 13.27 mg·g~(-1)(MB),and is dependent on adsorption time and initial dye concentration.The adsorption data for both dyes were well fitted to Freundlich isotherm model which explains the heterogeneous nature of TSAC surface.The dye adsorption obeyed pseudo-second order kinetic model,thus chemisorption was the controlling step.This study reveals potential of textile sludge in removal of dyes from aqueous solution,and further studies are required to establish the applicability of the synthesized adsorbent for the treatment of waste water containing toxic dyes from textile industry.     

容量法测量5 A分子筛静态吸附CH4、CO和CO2的研究

采用容量法分别测量CH₄、CO和CO₂在5A分子筛上的等温吸附曲线,探究吸附温度和吸附压力对CH₄、CO和CO₂吸附量的影响。实验结果表明,吸附量随着吸附压力的上升逐渐增大。设定吸附温度在30 ℃、50 ℃和70 ℃时,5A分子筛在30 ℃时对CH₄吸附量最大,为13.60 cm³·g^-1;对CO和CO₂吸附量均在50 ℃时呈现最大值,分别为17.68 cm³·g^-1 和94.38 cm³·g^-1。而吸附温度70 ℃时,对3种气体的吸附量均减小。     

Decorating MXene with tiny ZIF-8 nanoparticles: An effective approach to construct composites for water pollutant removal

MXenes have attracted increasing research enthusiasm owing to their unique physical and chemical properties. Although MXenes exhibit exciting potential in cations adsorption due to their unique surface groups, the adsorption capacity is limited by the low specific surface area and undeveloped porosity. Our work aims at enhancing the adsorption performance of a well-known MXene, Ti₃C₂T_x, for methylene blue (MB) by decorating tiny ZIF-8 nanoparticles in the interlayer. After the incorporation of ZIF-8, suitable interspace in the layers resulting from the distribution of tiny ZIF-8 appears. When employing in MB, the adsorption capacity of composites can reach up to 107 mg·g^-1 while both ZIF-8 (3 mg·g^-1) and Ti₃C₂T_x (9 mg·g^-1) show nearly no adsorption capacity. The adsorption mechanism was explored, and the good adsorption capacity is caused by the synergistic effect of ZIF-8 and Ti₃C₂T_x, for neither of them is of suitable interspace or surface groups for MB adsorption. Our work might pave the way for constructing functional materials based on the introduction of nanoparticles into layered materials for various adsorption applications.     

SnWO4/g-C3N4复合光催化剂降解亚甲基蓝溶液

采用溶剂热法制备SnWO_4/g-C_3N_4复合光催化剂,在可见光降解亚甲基蓝实验中研究复合催化剂的光催化性能。考察催化剂投加量、亚甲基蓝溶液初始浓度、溶液pH值、盐效应对光催化性能的影响及SnWO_4/g-C_3N_4复合光催化剂的重复利用性。实验结果表明,在催化剂投加量1.0 g·L~(-1)、亚甲基蓝溶液初始浓度15 mg·L~(-1)和溶液pH值7.08时,在可见光条件下反应3 h,亚甲基蓝溶液脱色率达到94.2%;NaCl对光催化降解亚甲基蓝具有抑制作用,加入10 mmol·L~(-1)的NaCl溶液后亚甲基蓝的脱色率降为76.0%;复合光催化剂循环使用5次后,暗吸附后光照3 h,亚甲基蓝溶液的总脱色率仍可达到78.7%,重复利用性良好。     

Synthesis of a novel functional group-bridged magnetized bentonite adsorbent:Characterization,kinetics, isotherm,thermodynamics and regeneration

A novel magnetic adsorbent was synthesized by magnetizing bentonite by APTES-Fe_3O_4 via a functional groupbridged interaction. The characterization of APTES-Fe_3O_4/bentonite was conducted via transmission electron microscope(TEM), X-ray diffraction(XRD), Fourier transform infrared spectrophotometer(FT-IR), thermal gravimetric analysis(TGA), vibrating sample magnetometer(VSM), zeta potential analysis and Brunner–Emmet–Teller(BET). The APTES-Fe_3O_4/bentonite was assessed as adsorbents for methylene blue(MB) with a high adsorption capacity(91.83 mg·g~(-1)). Factors affecting the adsorption of MB(such as p H, equilibrium time, temperature and initial concentration) were investigated. The adsorption process completely reaches equilibrium after 120 min and the maximum sorption is achieved at p H 8.0. The adsorption trend follows the pseudosecond order kinetics model. The adsorption data gives good fits with Langmuir isotherm model. The parameter factor RLfalls between 0 and 1, indicating the adsorption of MB is favorable. The adsorption process is endothermic with positive ΔH~0 values. The positive values of ΔG~0 confirm the affinity of the adsorbent towards MB, and suggest an increased randomness at the solid–liquid interface during the adsorption process. Regeneration of the saturated adsorbent was easily carried out via gamma-irradiation.     

MER型沸石吸附分离CO2/CH4的分子模拟

MER型沸石在吸附分离CO₂/CH₄方面展现出良好的工业应用前景，受到广泛关注，但还缺乏理论基础数据。本文采用巨正则蒙特卡洛（GCMC）模拟方法，以全硅MER型沸石作为对照，模拟分析了CO₂/CH₄在Na⁺、K⁺、Cs⁺和Ca²⁺交换的MER型沸石中的吸附分离行为。结果表明：不同阳离子交换的MER型沸石对CO₂和CH₄的吸附符合Langmuir-Freundlich吸附等温线模型，平衡吸附量的大小顺序为：Ca-MER＞Na-MER＞K-MER＞Cs-MER，与沸石的自由体积和比表面积大小顺序一致，且近似成线性关系，选用高价阳离子MER型沸石可以提高吸附量；CO₂和CH₄主要分布在沸石的pau笼中，在d8R笼和ste笼中也有少量分布；骨架外阳离子与CO₂的强吸附作用和独特的八元环窗口孔径是MER型沸石对CO₂/CH₄混合组分表现出超高吸附选择性的原因，吸附选择性高达1000以上。综合吸附量、吸附热和吸附选择性分析指出，Na-MER和K-MER型沸石是优良的CO₂吸附剂。本研究为MER型沸石吸附分离CO₂/CH₄提供了理论依据和实验指导。     

Preparation and evaluation of α-Al2O3 supported lithium ion sieve membranes for Li+ extraction

Spinel lithium manganese oxide ion-sieves have been considered the most promising adsorbents to extract Li⁺ from brines and sea water. Here, we report a lithium ion-sieve which was successfully loaded onto tubular α-Al₂O₃ ceramic substrates by dipping crystallization and post-calcination method. The lithium manganese oxide Li₄Mn₅O₁₂ was first synthesized onto tubular α-Al₂O₃ ceramic substrates as the ion-sieve precursor (i.e. L-AA), and the corresponding lithium ion-sieve (i.e. H-AA) was obtained after acid pickling. The chemical and morphological properties of the ion-sieve were confirmed by X-ray diffraction (XRD) and scanning electron microscopy (SEM). Both L-AA and H-AA showed characteristic peaks of α-Al₂O₃ and cubic phase Li₄Mn₅O₁₂, and the peaks representing cubic phase could still exist after pickling. The lithium manganese oxide Li₄Mn₅O₁₂ could be uniformly loaded not only on the surface of α-Al₂O₃ substrates but also inside the pores. Moreover, we found that the equilibrium adsorption capacity of H-AA was 22.9 mg·g^-1. After 12 h adsorption, the adsorption balance was reached. After 5 cycles of adsorption, the adsorption capacity of H-AA was 60.88% of the initial adsorption capacity. The process of H-AA adsorption for Li⁺ correlated with pseudo-second order kinetic model and Langmuir model. Adsorption thermodynamic parameters regarding enthalpy (ΔH), Gibbs free energy (ΔG) and entropy (ΔS) were calculated. For the dynamic adsorption- desorption process of H-AA, the H-AA exhibited excellent adsorption performance to Li⁺ with the Li⁺ dynamic adsorption capacity of 9.74 mg·g^-1 and the Mn²⁺ dissolution loss rate of 0.99%. After 3 dynamic adsorption-desorption cycles, 80% of the initial dynamic adsorption capacity was still kept.