氨基修饰的MCM-41和纯MCM-41的微波制备及去除废水中铜离子的研究

采用微波辅助水热法一步合成了具有大比表面积和孔径的氨基改性的MCM41(NH2-MCM41)和纯MCM-41,并用粉末X射线衍射、红外、氮气-吸脱附对其结构作了表征.将NH2-MCM-41和纯MCM-41用于吸附废水中的铜离子,其静态吸附实验表明:吸附量随温度的增加略有升高;铜离子在2种吸附剂上的吸附均符合Langmu...     

壳聚糖包覆介孔微孔分子筛去除水中的氨氮

以壳聚糖包覆介孔-微孔复合分子筛(CS/MCM-41-A)为吸附剂去除水中的氨氮,研究了反应时间、溶液p H、溶液氨氮初始浓度、CS/MCM-41-A投加量、竞争离子对吸附的影响,分析了CS/MCM-41-A的吸附动力学和热力学特征。结果表明,298 K下,当CS/MCM-41-A投加量为5 g/L,溶液氨氮初始浓度50 mg/L,p H为7,吸附时间为40 min时,溶液中氨氮的去除率达到74.35%,CS/MCM-41-A对离子的选择吸附顺序为Mg2+K+Ca2+Na+。CS/MCM-41-A吸附氨氮符合拟二级动力学方程,吸附等温线更好地符合Freundlich方程,CS/MCM-41-A对氨氮的去除有良好的吸附性能。     

巯基修饰MCM-41分子筛的制备及其对Cr(Ⅵ)的吸附动力学

以微硅粉为硅源,CTAB和PEG-6000为模板剂,制备得到MCM-41介孔分子筛,采用后接枝法将巯丙基三甲氧基硅烷引入到MCM-41的表面和孔道内,合成了巯基功能化的MCM-41介孔分子筛(SH-MCM-41)。采用TEM、N2吸附-脱附曲线、TG分析和XPS对样品进行了表征。以巯基功能化的样品为吸附剂,对含Cr(VI)的溶液进行了静态吸附实验,探讨了吸附过程的动力学。结果表明,SH-MCM-41对水中Cr(Ⅵ)的吸附经240 min可基本达到平衡,其理论吸附量为21.3 mg/g;利用准一级、准二级、Elovich方程、粒内扩散模型和班厄姆孔道扩散模型对吸附过程进行模拟,模拟结果表明,吸附过程符合准二级动力学模型,其拟合度R2为0.991,Elovich方程模拟相关系数R2大于0.95,表明吸附过程包含了多种反应机制。结果显示,吸附过程由液膜扩散、颗粒扩散和孔道扩散共同控制。     

MCM-41介孔分子筛的合成及其对铜离子的吸附性能

以微硅粉为硅源,CTAB和PEG-6000为模板剂,合成MCM-41介孔分子筛。采用XRD、N2吸附-脱附曲线、FT—IR以及TEM表征了其结构、比表面积、孔径分布及晶体形貌,并且以该样品为吸附剂,对含Cu2＋的溶液进行了静态吸附实验。结果表明,以微硅粉为硅源成功合成了具有典型六方排列孔道结构的MCM-41,其比表面积为869．5m。／g,孔容为0．97cm3／g,平均孔径为3．3nm;溶液pH为5—6时,MCM-41对Cu2＋的去除效果最好;MCM-41对Cu3＋的最大吸附吸附容量36．3mg／g;MCM-41对Cu2＋的吸附性能符合Langmuir吸附方程的特征。动力学研究表明,该过程符合准二级动力学模型。     

Pd/MCM-41对乙醇汽油车尾气排放乙醛的吸附和催化氧化性能

以正硅酸乙酯(TEOS)为硅源,十六烷基三甲基溴化铵(CTAB)为模板剂,采用水热合成法制备了MCM-41分子筛,以其为载体采用等体积浸渍法制得Pd/MCM-41催化剂,并用于乙醇汽油车冷启动排放乙醛的净化。采用氮气吸附脱附法(BET)、X射线衍射仪(XRD)、透射电子显微镜(TEM)对Pd/MCM-41理化性能进行表征,并用原位傅里叶变换红外技术研究了Pd/MCM-41在空气氛围下对乙醛的净化机理。结果表明:Pd/MCM-41具有规整的六方孔道、孔径分布均匀、比表面积大的特点;常温下,Pd/MCM-41催化剂可快速吸附乙醛,吸附容量可达105 mg·g~(-1),而吸附在Pd/MCM-41上的乙醛在180~220℃之间即可发生氧化而生成CO2和乙酸。     

MCM-41介孔分子筛的合成及其对铜离子的吸附性能简

以微硅粉为硅源,CTAB和PEG-6000为模板剂,合成MCM-41介孔分子筛。采用XRD、N₂吸附-脱附曲线、FTIR以及TEM表征了其结构、比表面积、孔径分布及晶体形貌,并且以该样品为吸附剂,对含Cu²⁺的溶液进行了静态吸附实验。结果表明,以微硅粉为硅源成功合成了具有典型六方排列孔道结构的MCM-41,其比表面积为869.5 m²/g,孔容为0.97 cm³/g,平均孔径为3.3 nm;溶液pH为5~6时,MCM-41对Cu²⁺的去除效果最好;MCM-41对Cu²⁺的最大吸附吸附容量36.3 mg/g;MCM-41对Cu²⁺的吸附性能符合Langmuir吸附方程的特征。动力学研究表明,该过程符合准二级动力学模型。     

酸碱盐改性对活性炭吸附油气特征的影响

采用酸碱盐溶液浸渍方法对活性炭进行改性,探究了其吸附油气的特征,考察了改性后的活性炭对油气吸附量和穿透时间的影响,采用BET、SEM、XRD及FT-IR等方法对活性炭进行了表征。结果表明:改性后的活性炭孔结构和表面化学性质发生了明显的变化,2~#样品(醋酸改性)比表面积最大为1 264.33 m~2·g~(-1),碱改性活性炭对油气的吸附性能优于其他改性方法,3~#样品(氨水改性)吸附容量最高为0.279 g·g~(-1),拟合动力学速率常数k′值是0.096 3,5#样品(氢氧化钾改性)穿透时间最长为130 min;改性处理后,增加了活性炭表面的—OH与C=C含量,正丁烷主要以—CH_2基团吸附在吸附剂表面。在综合酸碱盐溶液改性的基础上,利用Yoon-Nelson动力学方程对吸附曲线进行拟合,评价改性活性炭对油气的吸附性能。以上研究结果可为活性炭吸附油气的工业应用提供参考。     

改性硅藻土的制备及其对硝基苯的吸附性能研究

对硅藻土采用酸煮、碱煮和超声预处理,在不同温度下焙烧,然后用氢氧化铁改性得到9种改性硅藻土样品,并研究了改性后样品在不同pH、吸附剂的量、吸附时间、吸附温度下对硝基苯模拟废水的吸附性能。结果表明,酸煮后500℃焙烧下用氢氧化铁改性的硅藻土改性效果最好,并且在pH为5、吸附剂的量为1.0g(以硝基苯溶液250mL计)、吸附时间为120 min、温度为50℃时去除率最高,可达到99.5%,较未改性前提高了50百分点。     

硅烷化改性MCM-41负载戊二酸锌催化CO2与环氧丙烷共聚制备可降解材料

以三甲基氯硅烷(TMCS)为硅烷化试剂,对MCM-41分子筛进行表面改性处理,并以此为载体制备负载型戊二酸锌催化剂(ZnGA/TMCS-MCM-41);采用红外光谱、氮气吸附-脱附和X射线衍射等分析手段对催化剂进行表征,结果表明:三甲基氯硅烷基团被成功接枝到MCM-41分子筛表面,形成比表面积略低的硅烷化MCM-41载体,但其骨架未被破坏,负载活性物质过程中,戊二酸锌能以更小的粒径均匀分散到载体的表面;聚合反应实验表明,与单纯戊二锌催化剂相比,ZnGA/TMCS-MCM-41催化剂对CO2与环氧丙烷(PO)的共聚反应显示出更高的催化效率和更快的反应速度,在反应34 h后催化效率达到86.3 g聚合物/g ZnGA;红外光谱和核磁分析表明所得共聚产物中碳酸酯结构含量大于95.8%。     

QA-MCM-41吸附剂脱氮除磷性能

低浓度氮和磷在污水处理中较难去除,排放至水体会造成水体富营养化。以长碳链季铵为功能基团,将其接枝到自制备的介孔材料MCM-41上,成功制得一种吸附容量大且易再生的脱氮除磷吸附剂(QA-MCM-41)。采用SEM、XRD、BET等方法表征了QA-MCM-41微观形貌;研究了氮磷初始浓度、吸附时间及共存离子对QA-MCM-41吸附氮磷效果的影响;采用等温吸附模型、吸附动力学模型、ATR-IR以及XPS等分析手段探究了吸附反应机理。实验结果表明,QA-MCM-41对氮磷的饱和吸附量分别为20.83 mg·g~(-1)和17.67 mg·g~(-1),SO_4~(2-)对QA-MCM-41吸附氮磷的效果并未产生显著影响,吸附剂容易再生且重复利用性能较好。吸附动力学模拟及ATR-IR、XPS分析表明,QA-MCM-41对氮磷的吸附均符合以化学吸附为主导的准二级动力学方程,吸附作用主要依靠离子交换。     

Adsorption of basic dyes onto MCM-41

The adsorption of two basic dyes, Basic Green 5 (BG5) and Basic Violet 10 (BV10), onto MCM-41 was studied to examine the possible effect of interactions between large adsorbates and MCM-41 on the pore structure stability of MCM-41 and the potential of MCM-41 for the removal of basic dyes from wastewater. The revolutions of surface characteristics and pore structure of MCM-41 induced by dyes adsorption were characterized based on the analyses of the nitrogen isotherms, the XRD patterns, and the FTIR spectra. It was experimentally concluded that when the effect of interactions between large dyes (such as BV10) and MCM-41 on the pore structure stability of MCM-41 was insignificant, MCM-41 might be a good adsorbent for the removal of basic dyes from wastewater. The adsorption of BV10 on MCM-41 with respect to contact time, pH, and temperature was then measured to provide more information about the adsorption characteristics of MCM-41. Both Langmuir and Freundlich adsorption models were applied to describe the equilibrium isotherms and the pseudo-second-order kinetic model was used to describe the kinetic data, from which some adsorption thermodynamic parameters were also evaluated.     

天然及CaCl2改性沸石对四环素的吸附

通过静态吸附实验研究了水中四环素在天然和CaCl2改性沸石上的吸附行为及机制。实验表明,天然沸石对四环素具有吸附能力,CaCl2改性可以提高沸石对四环素的吸附能力。天然和改性沸石对四环素的吸附符合拟二级动力学模型,颗粒内扩散不是吸附过程的主要控制步骤。Freundlich和Dubinin-Radushkevich(D-R)等温吸附模型可以较好地描述实验所用2种沸石对四环素的吸附行为,D-R等温方程拟合结果显示吸附过程包含离子交换作用。通过对天然和改性沸石吸附四环素前后溶液中主要阳离子浓度变化分析证实了该吸附过程包含离子交换作用。实验研究了pH值变化对沸石吸附四环素的影响,当pH=3～5时,天然和改性沸石对四环素的吸附量均随pH值的增加而急剧下降,而pH=5～10时,天然和改性沸石对四环素的吸附量变化均不明显,推测可能是离子交换作用和化学沉淀吸附作用所致。另外,实验还初步探索了溶液离子强度对沸石吸附四环素的影响情况,随着溶液中Na+和Ca2+离子强度的增加,吸附量先急剧降低随后趋向平稳,进一步说明了沸石对四环素的吸附过程不是由单一机制控制的。     

天然及CaCl_2改性沸石对四环素的吸附

通过静态吸附实验研究了水中四环素在天然和CaCl2改性沸石上的吸附行为及机制。实验表明,天然沸石对四环素具有吸附能力,CaCl2改性可以提高沸石对四环素的吸附能力。天然和改性沸石对四环素的吸附符合拟二级动力学模型,颗粒内扩散不是吸附过程的主要控制步骤。Freundlich和Dubinin-Radushkevich（D-R）等温吸附模型可以较好地描述实验所用2种沸石对四环素的吸附行为,D-R等温方程拟合结果显示吸附过程包含离子交换作用。通过对天然和改性沸石吸附四环素前后溶液中主要阳离子浓度变化分析证实了该吸附过程包含离子交换作用。实验研究了pH值变化对沸石吸附四环素的影响,当pH=3～5时,天然和改性沸石对四环素的吸附量均随pH值的增加而急剧下降,而pH=5～10时,天然和改性沸石对四环素的吸附量变化均不明显,推测可能是离子交换作用和化学沉淀吸附作用所致。另外,实验还初步探索了溶液离子强度对沸石吸附四环素的影响情况,随着溶液中Na＋和Ca2＋离子强度的增加,吸附量先急剧降低随后趋向平稳,进一步说明了沸石对四环素的吸附过程不是由单一机制控制的。     

Adsorption of mesitylene via mesoporous adsorbents

Mesitylene (or 1,3,5-trimethylbenzene) is a volatile organic compound emitted from various industrial processes, e.g., spray coating. Its emissions have become a critical issue because mesitylene is toxic and cannot be removed using traditional adsorbents, e.g., zeolite (H-ZSM-5; the diameter of mesitylene molecules is greater than the pore size of H-ZSM-5). Hence, an adsorbent with a large pore size, MCM-41, is used in this study to investigate its adsorption capacity for mesitylene and compare with that of H-ZSM-5. Experimental results reveal that MCM-41 without Al₂O₃ exhibits a good adsorption capacity (184 mg/g) for the gas stream containing 100 ppm of mesitylene at a relative humidity of 10%. The adsorption kinetics is well described by the Freundlich isotherm. Furthermore, experimental results reveal that MCM-41 is effective for the adsorption of low concentrations (10 ppm) of mesitylene. In addition, adsorption–desorption tests revealed that the sample MCM-41-AS is stable to sustain the adsorption capacity after 10 adsorption–desorption cycles. After 10 adsorption–desorption cycles, MCM-41-AS retains 92.4% of its initial adsorption capacity (170 vs. 184 mg/g). Finally, MCM-41 and H-ZSM-5 in series are effective for the simultaneous removal of mesitylene and toluene in the gas stream.

Implications: This study aims to improve the performance of adsorbent for mesitylene, which is typically applied in the spray-coating industry. The zeolite MCM-41-AS is selected as a candidate for the investigation. Experimental results reveal that MCM-41-AS exhibits a good adsorption capacity for mesitylene and that it can be integrated with H-ZSM-5-25 for the simultaneous adsorption of mesitylene and toluene.     

Competitive adsorption characteristics of Co2+, Ni2+, and Cr3+ by IRN-77 cation exchange resin in synthesized wastewater

Adsorption properties of Co2+, Ni2+, and Cr3+ on an Amberlite IRN-77 cation exchange resin were investigated in batch systems. Levels of adsorption rapidly approached an equilibrium state within 1 h. The adsorption characteristics of each metal onto the resin were accurately represented by Langmuir isotherms. Co2+ and Ni2+, which have an equivalent electrovalence, displayed similar levels of adsorption onto the resin when they coexisted in the solution. However, when Cr3+ was added to the solution it competitively replaced Co2+ and Ni2+ ions that had been previously adsorbed onto the resin, resulting in the desorption of these metals into the solution. The result was likely due to a higher adsorption affinity of Cr3+ relative to Co2+ and Ni2+. This implies that interactively competitive adsorption of multi-cations onto the resin should be thoroughly considered when contemplating the efficient operation of an ion exchange process in the treatment of industrial wastewater.     

季铵化合物对好氧活性污泥吸附Ni2+的影响研究

以季铵化合物中最具潜在影响力、毒性较大的苄基季铵盐(BAC)为模型物,进行了BAC对好氧活性污泥吸附Ni2+的影响研究.结果表明,当反应液初始pH≤3时,不同浓度的BAC对好氧活性污泥吸附Ni2+的影响较小,当初始pH在3～9时,不同浓度的BAC对Ni2+吸附的抑制影响顺序为100 mg/L＞20 mg/L＞0 mg/...     

Carbon dioxide adsorption on amine-impregnated mesoporous materials prepared from spent quartz sand

Mesoporous MCM-41 was synthesized using cetyltrimethyl ammonium bromide (CTAB) as a cationic surfactant and spent quartz sand as the silica source. Modification of the mesoporous structure to create an absorbent was then completed using 3-aminopropyltrimethoxysilane. Amine-Quartz-MCM (The A-Q-MCM) adsorbents were then characterized by N₂ adsorption/desorption, elemental analysis (EA), X-ray fluorescence (XRF), scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FTIR), as well as the carbon dioxide (CO₂) adsorption/desorption performance. In this study, spent quartz sand was utilized to synthesize Quartz-MCM (Q-MCM) and the amine functionalized material, A-Q-MCM, which exhibited a higher uptake of CO₂ at room temperature compared with the nongrafted material. The results showed that Q-MCM is similar to MCM-41 synthesized using commercial methods. The surface area, pore volume, and pore diameter were found to be as high as 1028 m²/g, 0.907 cm³/g, and 3.04 nm, respectively. Under the condition of CO₂ concentration of 5000 ppm, retention time of 50 cc/min, and the dosage of 1 g/cm³, the mean adsorption capacity of CO₂ onto A-Q-MCM was about 89 mg/g, and the nitrogen content of A-Q-MCM was 2.74%. The adsorption equilibrium was modeled well using a Freundlich isotherm.

Implications:In this study, spent quartz sand was utilized to synthesize Q-MCM. The amine functionalized material exhibited a higher uptake of CO₂ at room temperature compared with the nongrafted material. The results showed that Q-MCM is similar to MCM-41 synthesized using commercial methods. The adsorption equilibrium was modeled well using a Freundlich isotherm.     

Fate of nickel in a lime-stabilized biosolid,a calcareous soil and soil–biosolid mixtures

Soil contamination with anthropogenic metals resulting from biosolid application is widespread around the world. To better predict the environmental fate and mobility of contaminants, it is critical to study the capacity of biosolid-amended soils to retain and release metals. In this paper, nickel adsorption onto a calcareous soil, a lime-stabilized biosolid, and soil–biosolid mixtures (30, 75, and 150 t biosolid/ha) was studied in batch experiments. Sorption experiments showed that (1) Ni adsorption was higher onto the biosolid than the calcareous soil, and (2) biosolid acted as an adsorbent in the biosolid–soil mixtures by increasing Ni retention capacity. The sorption tests were complemented with the estimation of Ni adsorption reversibility by successive applications of extraction solutions with water, calcium (100 mg/L), and oxalic acid (equivalent to 100 mg carbon/L). It has been shown that Ni desorption rates in soil and biosolid-amended soils were lower than 30 % whatever the chemical reagent, indicating that Ni was strongly adsorbed on the different systems. This adsorption/desorption hysteresis effect was particularly significant at the highest biosolid concentration (150 t/ha). Finally, an adsorption empirical model was used to estimate the maximum permissible biosolid application rate using French national guideline. It has been shown that desorption effects should be quantitatively considered to estimate relevant biosolid loadings.