SAPO-34分子筛的动态吸附特性实验研究

对于吸附式制冷系统而言,吸附材料的选择是系统的核心问题。对两种不同厂家的SAPO-34沸石分子筛进行了吸附特性测试。其共同特性是,温度一定时,SAPO-34分子筛的吸附量随相对湿度的增加而增大。相对湿度在40%~60%时,吸附量变化不大;而相对湿度在70%~80%时,吸附量增加较快。另一方面,由于两种SAPO-34样品的微观结构有一定差异,导致其吸附量和吸附速率也不一样。粒径较小、孔隙率较大的样品A,其吸附量比样品B大1~2倍,达到吸附饱和的时间也缩短近100分钟。此特性有利于改善吸附制冷系统的整体性能。     

基于傅里叶红外光谱的生物质环境协调功能材料制备机理及性能研究

以废弃核桃壳为载体材料、癸酸为相变材料,采用微波加热法制备癸酸/多孔活性炭功能材料。采用傅里叶红外光谱仪对癸酸/多孔活性炭功能材料制备过程各阶段的合成物质进行测试,即活性炭前驱体制备阶段、多孔活性炭制备阶段和癸酸/多孔活性炭功能材料制备阶段。研究癸酸/多孔活性炭功能材料制备过程中多孔活性炭复杂网络结构形成机理、癸酸嵌入方式、癸酸与多孔活性炭的嵌合机理,阐明微波加热法制备癸酸/多孔活性炭功能材料的相关机理。同时采用动态水分吸附分析仪、差示扫描量热仪和环境测试舱对癸酸/多孔活性炭功能材料的湿性能、热性能和吸附性能进行测试。结果表明：癸酸/多孔活性炭功能材料具有发达的孔结构和复杂的网络结构,其中部分孔隙吸附癸酸,部分孔隙吸附甲醛分子,孔隙表面具有亲水性的官能团吸附水分子。癸酸/多孔活性炭功能材料具有较好的湿性能、热性能和吸附性能,其在相对湿度40%~60%,平衡含湿量为0.063 1~0.257 0 g·g-1;相变温度为27.42~33.96 ℃,相变焓为52.14~52.67 J·g-1;经过4 h对甲醛气体的吸附效率为50.57%。     

非固结多孔介质干燥的双尺度孔道网络模型与模拟

以农产品颗粒物料中常见孔隙直径范围(10~(-4)～10~(-3) m)的非固结多孔介质为研究对象,运用孔道网络方法和传递过程原理等知识,建立了考虑骨架吸湿、汽相对流、温度梯度和孔道结构特征等因素对干燥过程影响的非固结多孔介质双尺度孔道网络干燥模型,并进行了相应的干燥实验.模拟与实验结果表明:该模型可有效模拟非固结多孔介质的干燥过程;非固结多孔介质的孔隙率、直径(包括粒径与孔径)分布对干燥的影响十分显著,孔隙率越大,物料干燥越快,达到相同湿含量干燥所需时间越短;直径分布的不均匀程度越高,干燥所需时间越长,物料湿含量分布的差异也越大。对于窄筛分农产品颗粒物料,进行干燥计算时可以采用同一直径分布代替实际分布.     

ICP-OES研究活性炭无纺布对镉的吸附

重金属污染是一个相当严重的环境问题。镉具有很强的生物毒性和不可降解性,对生态环境和人体健康有极大威胁,被列为优先控制污染物。环境中镉的主要污染源是电镀、采矿和化学工业等部门的废水,如何简单高效去除水中的镉,有重要的社会意义和经济意义。目前,水中重金属的去除方法有化学沉淀、膜分离、离子交换、吸附、电解等,其中吸附法因简单高效而广泛应用。活性炭纤维是一种新型活性炭,孔径小且均匀,表面官能团发达,吸附性能好,逐步应用于水处理领域。以电感耦合等离子体光谱为检测手段,佐以比表面积分析,X射线衍射,元素分析和傅里叶变换红外光谱,研究比较了三种活性炭纤维(纤维炭网、活性炭无纺布、活性炭纤维毡)的结构特点及其对水中镉的吸附性能。三种活性炭纤维结构基本类似,具有较发达的孔隙结构。活性炭无纺布极性较强,表面有丰富的羟基、羧基、醛基等含氧官能团,对水中镉的吸附作用最大。因此,选择活性炭无纺布为吸附剂进行后续实验。研究了活性炭无纺布吸附镉的影响因素,如溶液pH,吸附时间等。溶液pH影响吸附剂表面电荷及水中镉的存在状态。水中镉的去除效率随溶液初始pH的增大而增大,在较低pH时,吸附剂与Cd2+间存在静电斥力,同时H+和Cd2+存在竞争吸附,pH>9时,镉的去除是吸附与沉淀协同作用的结果,选择pH为6～7。在吸附的初始阶段,活性炭无纺布对Cd2+的吸附量迅速增加,10 min时,吸附率达到72%。随着吸附位点逐渐被Cd2+所填充,吸附速率逐渐变慢,300 min时,吸附容量基本无变化,吸附趋于平衡。优化了镉的吸附条件后,进行等温吸附实验和动力学实验。结果表明,25 ℃时,吸附时间为300 min,pH 6.0条件下,当镉的平衡浓度在20.00 mg·L-1时,活性炭无纺布对镉的单位质量吸附量和单位比表面积吸附量分别是3.04 mg·g-1和0.035 mg·m-2。用Langmuir方程(R2=0.997, K_L =1.796 L·mg-1)和Freundich方程(R2=0.895, K_F=0.918 L·mg-1, n=2.12)拟合活性炭无纺布对镉的等温吸附数据,Langmuir方程计算的理论吸附量为3.07 mg·g-1,与实验值相当,并且线性系数更高,说明该体系的吸附符合Langmuir方程,主要为单分子层吸附。Langmuir分离因子介于0和1之间,表明活性炭无纺布对镉的吸附容易进行。用准一级动力学方程、准二级动力学方程、颗粒内扩散方程和Elovich方程四种动力学模型拟合吸附过程。在吸附的前5 min,镉在活性炭无纺布上的吸附符合颗粒内扩散方程(R2=0.985),吸附主要受颗粒内扩散控制。在吸附的5～300 min,颗粒内扩散方程拟合较差。整个吸附过程符合准二级动力学方程(R2=0.999,k₂=0.367 g·mg-1·min-1),Elovich方程(R2=0.981,a=0.271 mg·g-1, b=0.083 mg·g-1·(lg min)-1)和准一级动力学方程(R2=0.927,k₁=0.008 8 min-1)次之,颗粒内扩散方程(R2=0.785)最差。活性炭无纺布对镉的吸附过程是一种化学作用为主的吸附过程。对5.00 mg·L-1含镉水样,活性炭无纺布投放量为10 g·L-1时,吸附后水中镉的浓度小于0.10 mg·L-1,符合《污水综合排放标准》(GB 8978-1996)。活性炭无纺布可同时吸附镉,铜,铅,铬等重金属离子,选择性较差。但在电镀、采矿等实际废水中重金属种类复杂,适当提高吸附剂投放量,可同时去除多种重金属。利用活性炭无纺布吸附处理含镉水样,处理效果好、操作简单,可以作为去除水中镉的吸附剂,为含镉废水的处理提供了技术支持和理论基础。     

CO2地质封存中突破压力梯度的孔隙尺度数值模拟

以CO2捕集与封存为研究背景,开展了二氧化碳盐水层封存条件下超临界二氧化碳在多孔结构中的流动规律研究.通过基于孔隙尺度的数值模拟方法,研究了超临界CO2注入储层多孔结构时突破压力梯度和流动时间以及CO2饱和度的关系,分析了压力、温度、颗粒直径、接触角和表面张力系数对突破压力梯度的影响规律.研究表明,对于孔隙率以及颗粒分...     

溴素改性活性炭汞吸附特性研究

在固定床实验台上进行了1%NH_4Br改性活性炭汞吸附实验。利用吸附动力学模型从动力学角度探讨了汞吸附速率控制步,汞吸附活化能与初始汞吸附速率。结果表明:150℃时,1%NH_4Br改性活性炭脱汞能力显著增强,其原因是改性后活性炭表面活性位点(Br)明显增加,强化了化学吸附作用。但低温时,化学吸附增强作用不明显。汞在改性活性炭表面的吸附活化能为29.69 kJ/mol,说明吸附以物理吸附为主,化学吸附为辅。改性活性炭的初始汞吸附速率随温度增加而增加。活性位吸附是汞吸附速率控制步,外部传质控制也影响整个汞吸附过程,吸附遵循Langmuir吸附等温方程。     

基于二氧化钛-介孔硅复合材料的光催化毒气过滤器

介绍了一种介孔硅与纳米二氧化钛的复合方法,制备了兼具高吸附性与高光催化活性的纳米二氧化钛-介孔硅复合材料.在此基础上,以365nm波长的紫外LED为光源、特制的半泄露聚合物光纤为导光介质制造了一种新型的光催化毒气过滤器.实验结果表明:当LED光功率为540mW,复合材料装填量为350g时,该过滤器对甲醛气体的吸附量大于3mg;当过滤器达吸附饱和后,输入甲醛气流量为2L/min、浓度为0.7mg/m~3,实时分解甲醛的速率达72μg/h,输出气体中甲醛浓度降至0.09mg/m~3,低于国家卫生标准中的室内甲醛浓度的安全阈值.纳米二氧化钛-介孔硅复合光催化剂的吸附特性为光催化分解提供了充分的反应时间,有利于提高光催化分解效率,可以长时间循环工作,有望用于家庭空气净化,甚至取代现有的活性炭过滤器,用在长效的防毒面具等装置中.     

基于电化学-热耦合模型研究隔膜孔隙结构对锂离子电池性能的影响机制

隔膜孔隙结构对锂离子电池性能具有重要的影响,本文提出了可准确描述充放电过程中锂离子电池内部复杂物理化学现象的电化学-热耦合模型,发现该模型较文献中模型的计算结果更接近实验测试数据.利用该模型探讨了隔膜孔隙率与扭曲率分别对锂离子电池性能的影响规律,发现减小孔隙率或增大扭曲率,电池输出电压、最大放电容量和平均输出功率均不断降低,电池表面温度和温升速度均不断升高;当孔隙率减小或扭曲率增大到一定程度时,放电初期电池输出电压均会出现先下降后回升的现象,且孔隙率越小或扭曲率越大,其下降的幅度越大、速度越快,回升所需时间也越长;要确保其不低于截止电压,隔膜扭曲率必须小于临界扭曲率(其下降至最低点刚好等于截止电压时的隔膜扭曲率).综合分析了放电过程中电池内部各电化学参量和产热量的动态分布规律,发现隔膜孔隙率和扭曲率主要影响放电末期电极膜片内部电化学反应以及其他放电时刻电解液中有效Li~+扩散(传导)系数.     

纸质活性炭纤维的制备及性能表征

通过KOH活化纸巾制备活性炭纤维, 比表面积高达1388 m²/g. 用制得的活性炭纤维作为吸附剂进行亚甲基蓝吸附实验研究,用Langmuir和Freundlich吸附模型分析实验数据,并研究pH值对活性炭纤维吸附亚甲基蓝影响. 活性炭纤维吸附速率更适于Pseudo-second-order动力学模型,相关系数高达0.998. 整个浓度变化区间Langmuir吸附等温线比Freundlich吸附等温线更适合实验数据. 所制备活性炭纤维对亚甲基蓝最大平衡吸附量为520 mg/g,实验发现,pH值越高活性炭纤维对亚甲基蓝吸附量越大.     

活性炭表面含氧官能团对汞吸附的作用

本文对采用不同方法处理后的活性炭进行BET、官能团分析和汞吸附性能实验,研究其表面含氧官能团对汞吸附的作用。结果表明:活性炭表面的酯基与羰基能提高汞的吸附效率,高于100℃时是影响活性炭汞吸附效率的主要因素。物理吸附,羰基与酯基吸附的汞的程序升温脱附温度峰值分别为100,210和320℃。汞在与活性炭表面接触后优先被吸附能高的化学吸附位点吸附,化学吸附饱和后,才会进行物理吸附。     

Characterization of partially sintered ceramic powder compacts using fluorinated gas NMR imaging.

We use nuclear magnetic resonance (NMR) imaging of C2F6 gas to characterize porosity, mean pore size, and permeability of partially sintered ceramic (Y-TZP Yttria-stabilized tetragonal-zirconia polycrystal) samples. Conventional measurements of these parameters gave porosity values from 0.18 to 0.4, mean pore sizes from 10 nm to 40 nm, and permeability from 4 nm(2) to 25 nm(2). The NMR methods are based on relaxation time measurements (T(1)) and the time dependent diffusion coefficient D(Delta). The relaxation time of C2F6 gas is longer in pores than in bulk gas and it increases as the pore sizes decrease. NMR yielded accurate porosity values after correcting for surface adsorption effects. A model for T(1) dependence on pore size that accounts for collisions between gas molecules and walls as well as surface adsorption effects is proposed. The model fits the experimental data well. Finally, the long time limit of D(Delta)/D(o), where D(o) is the bulk gas diffusion coefficient is useful for measuring tortuosity, while the short time limit was not achieved experimentally and could not be used for calculating surface-area to volume (S/V) ratios.     

Surface heterogeneity effects of activated carbons on the kinetics of paracetamol removal from aqueous solution

The removal of a compound with therapeutic activity (paracetamol) from aqueous solutions using chemically modified activated carbons has been investigated. The chemical nature of the activated carbon material was modified by wet oxidation, so as to study the effect of the carbon surface chemistry and composition on the removal of paracetamol. The surface heterogeneity of the carbon created upon oxidation was found to be a determinant in the adsorption capability of the modified adsorbents, as well as in the rate of paracetamol removal. The experimental kinetic data were fitted to the pseudo-second order and intraparticle diffusion models. The parameters obtained were linked to the textural and chemical features of the activated carbons. After oxidation the wettability of the carbon is enhanced, which favors the transfer of paracetamol molecules to the carbon pores (smaller boundary layer thickness). At the same time the overall adsorption rate and removal efficiency are reduced in the oxidized carbon due to the competitive effect of water molecules.     

Factors influencing activated carbon-polymeric composite membrane structure and performance

Hybrid carbon-polymeric composite membranes were synthesized by an immersion-precipitation method using polysulfone as polymer precusor and activated carbon dissolved in dimethyl formamide as casting solution. Surface analysis by scanning electron microscopy (SEM) allowed studying the morphology of membranes as a function of synthesis conditions (carbon loading and particle size). Membrane porosity distribution and mean pore size were obtained numerically using IFME^® program.Effect of casting conditions over carbon was also investigated by SEM.Hybrid membrane performances were characterized in terms of water and oligomeric flux in a continuous operation mode. Selective rejection of dextranes of high molecular weight was obtained. Results showed that permeability for composite membranes is influenced basically by loading and activated carbon particle size, giving rise to materials with a better performance than non-hybrid ones for this application.     

Cellulose Acetate/Activated Carbon Composite Membrane with Effective Dye Adsorption Performance

Abstract

Cellulose acetate (CA) and activated carbon (AC) were used as base material and additive, respectively, to prepare CA/AC composite membranes. By adjusting the AC content (5%, 10%, 15%, and 20%), the morphology and the adsorption capability of the samples for target dyes were studied. The results showed that the surface flatness and compactness of the barrier layer deteriorated with increasing AC content. In addition, the pore size and structures of the supporting layer became large due to the partial agglomeration of the AC in the CA. The relationship between adsorption time and adsorption capability was investigated. It was found that the 15% AC composite membrane possessed the highest adsorption efficiency for acid blue dye. The adsorption equilibrium was 58.69?mg/g for 60?mg/L acid blue dye at 120?min. For acid yellow and acid dark dye, the adsorption equilibria were 58.23 and 58.34?mg/g, respectively.     

Calculation method for particle mean diameter and particle size distribution function under dependent model algorithm

In total light scattering particle sizing technique, the relationship among Sauter mean diameter D32, mean extinction efficiency Q, and particle size distribution function is studied in order to inverse the mean diameter and particle size distribution simply. We propose a method which utilizes the mean extinction efficiency ratio at only two selected wavelengths to solve D32 and then to inverse the particle size distribution associated with (Q) and D32. Numerical simulation results show that the particle size distribution is inversed accurately with this method, and the number of wavelengths used is reduced to the greatest extent in the measurement range. The calculation method has the advantages of simplicity and rapidness.     

随机四参数法生成多孔介质及渗流模拟

本文基于多孔介质内流动的广泛应用背景,模拟了多孔介质渗流。采用随机四参数生长法生成了多孔介质模型,并对模型中的微小固相进行了过滤处理。将随机四参数生长法生成的多孔介质结合格子玻尔兹曼方法D2Q9模型模拟了压力驱动的多孔介质中的渗流。通过将模拟结果与著名的CK理论公式的计算结果进行比较,发现在孔隙率高时误差较小(φ=0.9时,误差约为6%)。研究表明在高孔隙率时采用文中的方法得到的多孔介质渗透率及孔隙尺度的流动结果较为准确。     

Coalbed methane adsorption and desorption characteristics related to coal particle size

Effects of particle size on CH_4 and CO_2adsorption and desorption characteristics of coals are investigated at 308 K and pressures up to 5.0 MPa.The gas adsorption and desorption isotherms of coals with particle sizes ranging from 250 μm to 840 μm are measured via the volumetric method,and the Langmuir model is used to analyse the experimental results.Coal particle size is found to have an obvious effect on the coal pore structure.With the decrease of coal particle size in the process of grinding,the pore accessibility of the coal,including the specific surface area and pore volume,increases.Hence,coal with smaller particle size has higher specific surface area and higher pore volume.The ability of adsorption was highly related to the pore structure of coal,and coal particle size has a significant influence on coal adsorption/desorption characteristics,including adsorption capacity and desorption hysteresis for CH_4 and CO_2,i.e.,coal with a smaller particle size achieves higher adsorption capacity,while the sample with a larger particle size has lower adsorption capacity.Further,coal with larger particle size is also found to have relatively large desorption hysteresis.In addition,dynamic adsorption performances of the samples are carried out at 298 K and at pressures of 0.1 MPa and 0.5 MPa,respectively,and the results indicate that with the increase of particle size,the difference between CO_2 and CH_4adsorption capacities of the samples decreases.     

孤立碳颗粒聚团燃烧过程的研究

数值模拟气体流过孤立碳颗粒聚团的燃烧反应过程。计算表明穿过颗粒聚团的气体流量主要与颗粒聚团空隙率有关。当颗粒聚团空隙率小于0．8时,穿过颗粒聚团的气体流量可忽略不计。碳颗粒聚团内温度呈现迎来流面低、背流面高,两侧低中间高; CO和CO2含量呈现迎来流面低、背流面高,两侧低中间高的变化趋势;而O2含量迎来流面高、背流面低,两侧高中间低。颗粒聚团内不同位置的颗粒消耗的碳量不同。颗粒的相互团聚将降低碳的消耗量,同时也抑制碳颗粒燃烧过程NO和N2O的生成。     

Surface effect on the size evolution of surface plasmon resonances of Ag and Au nanoparticles dispersed within mesoporous silica

The optical absorption has been investigated for silver and gold nanoparticles dispersed within the pores of monolithic mesoporous silica after annealing at different temperatures. It has been shown that with reduction of the particle size, the surface plasmon resonance position blue-shifts first and then red-shifts for silver/silica samples, but only red-shifts for gold/silica samples. This size evolution of the resonance is completely different from that previously reported for fully embedded particles. Based on the interaction of the particle surface with ambient air and the porosity at the particle/matrix interface, we present a multi-layer core/shell model and assume that the chemical adsorption of gas molecules from the air on the free surface of nanoparticles within the pores is mainly responsible for the observed size evolution of the resonance.