两种ZSM-5沸石分子筛吸附水中氨氮的研究

考察了两种硅铝比分别为25及50的ZSM-5沸石分子筛对水中氨氮的吸附性能及影响因素.研究表明,25℃时,25H及50H型沸石的吸附平衡时间分别为10 min和35 min,吸附等温线均符合Langmuir经验模型,25 H型分子筛的饱和吸附容量较大,为7.83 mg/g,50H型分子筛为4.36 mg/g.当吸附剂投...     

钴铜改性的ZSM-5对低浓度NO吸附性能的研究

利用固定吸附床研究了不同金属离子改性的ZSM-5分子筛对一氧化氮的吸附性能。实验发现:在过渡金属同钴离子一起改性的ZSM-5中,钴铜金属离子共同改性的ZSM-5分子筛对一氧化氮的吸附性能最好;当铜钴离子共同浸渍、铜钴离子浸渍量比(n(Cu) n(Co))为0 8和Al2O3(粘合剂)用量w(Al2O3)为23%时,改性的ZSM-5分子筛既具有良好的吸附性能又有良好的机械强度。另外,实验还发现改性分子筛吸附一氧化氮的穿透时间随吸附温度的升高而缩短,并利用热重技术,分析了吸附剂的热再生问题。      

Application of high silica zeolite ZSM-5 in a hybrid treatment process based on sequential adsorption and ozonation for VOCs elimination

In this study, a hydrophobic synthetic zeolite, namely ZSM-5 is chosen as an adsorbent/catalyst for toluene removal. Experimental results showed that toluene adsorption onto ZSM-5 was favourable, following a Langmuir adsorption isotherm model. ZSM-5 zeolite was regenerated using gaseous ozone at low temperature. Adsorbed toluene was oxidised, releasing mainly CO₂ and H₂O. Traces of oxidation by-products such as acetic acid and acetaldehyde were formed and remained adsorbed after the oxidativate regeneration with ozone. After four successive cycles of adsorption/ozonation, the adsorption efficiency was not affected (92%–99%). These results showed that volatile organic compound (VOC) removal by adsorption onto ZSM-5 zeolite followed by ozone regeneration could be used as a promising hybrid process for the control of VOC emissions in terms of efficiency.     

硅铝比和NiO对ZSM-5协同低温等离子体降解甲苯的影响

研究了不同硅铝比的ZSM-5与Ni/ZSM-5分子筛协同低温等离子体技术对甲苯降解性能的影响.以Ni O(Nickel Oxide)为活性组分,采用浸渍法对ZSM-5分子筛进行改性,利用氮气吸附脱附(BET)、X射线衍射仪(XRD)、X射线光电子能谱分析(XPS)、H_2程序升温还原(H_2-TPR)、NH_3程序升温脱附(NH_3-TPD)、Toluene程序升温脱附(Toluene-TPD)等技术表征样品的物理化学性质.考察了硅铝比对ZSM-5与Ni/ZSM-5分子筛体系中甲苯的吸附性能,研究了不同放电电压下硅铝比对甲苯降解率、碳平衡及二氧化碳选择性的影响,并采用气相色谱-质谱联用仪(GC-MS)分析了催化剂表面的有机产物.结果表明:硅铝比不但影响分子筛本身的物理化学特性(比表面积、氧化还原性能、表面酸性、疏水性等),还会影响Ni的负载形态和方式,更高的硅铝比与Ni O的负载能促进甲苯深度氧化,减少副产物,提高碳平衡和二氧化碳选择性.     

Effects of metal cations on sorption-desorption of p-nitrophenol onto wheat ash

The mutual e ects of metal cations (Cu2+, Pb2+, Zn2+, and Cd2+) and p-nitrophenol (NP) on their adsorption desorption behavior onto wheat ash were studied. Results suggested that Cu2+, Pb2+, and Zn2+ diminished the adsorption and increased the desorption of NP remarkably, while Cd2+ had no such e ect. In contrast, NP diminished the adsorption of Cu2+, Pb2+, and Zn2+ onto ash, however, this suppression e ect depended on the initial concentrations of metal cations. NP had no e ect on Cd2+ adsorption on ash. Fourier transform infrared (FT-IR) and X-ray absorption spectroscopic (XAS) studies suggested the following mechanisms responsible for the metal suppression e ect on NP adsorption: (1) large hydrated Cu2+, Pb2+, and Zn2+ shells occupied the surface of ash and prevent nonspecific adsorption of NP onto ash surface; (2) Cu2+, Pb2+, and Zn2+ may block the micropores of ash, resulting in decreased adsorption of NP; (3) complexation of Cu2+, Pb2+, and Zn2+ was likely via carboxyl, hydroxylic and phenolic groups of wheat ash and these same groups may also react with NP during adsorption. As a “soft acid”, Cd2+ is less e cient in the complexation of oxygencontaining acid groups than Cu2+, Pb2+, and Zn2+. Thus, Cd2+ had no e ect on the adsorption of NP on wheat ash.     

水钠锰矿的Mn（Ⅲ）分布及Na4P2O7溶液处理对其铅吸附性能的影响

以深入理解水钠锰矿结构中低价锰离子的含量及分布对其铅吸附性能的影响为目的,通过不同pH（pH为2、4、5）的焦磷酸钠溶液络合浸提酸性水钠锰矿结构中的Mn（Ⅱ）和Mn（Ⅲ）,研究了浸提锰离子的形态、含量、矿物的锰平均氧化度和Pb2＋的吸附量及其伴随Mn2＋、H＋释放量的变化.结果表明,锰平均氧化度为3.670的酸性水钠锰...     

Adsorption of acetanilide herbicides on soil and its components. II. Adsorption and catalytic hydrolysis of diethatyl-ethyl on saturated Na(+)-, K(+)-, Ca(2+)-, and Mg(2+)-montmorillonite

Adsorption and catalytic hydrolysis of the herbicide diethatyl-ethyl [N-chloroacetyl-N-(2,6-diethylphenyl)glycine ethyl ester] on homoionic Na⁺-, K⁺-, Ca²⁺-, and Mg²⁺-montmorillonite clays were investigated in water solution. The Freundlich adsorption coefficient, Kf, got from isotherms on clay followed the order of Na⁺ K⁺ > Mg²⁺ Ca²⁺. Analysis of FT-IR spectra of diethatyl-ethyl adsorbed on clay suggests probable bonding at the carboxyl and amide carbonyl groups of the herbicide. The rate of herbicide hydrolysis in homoionic clay suspensions followed the same order as that for adsorption, indicating that adsorption may have preceded and thus caused hydrolysis. Preliminary product identification showed that hydrolysis occurred via nucleophilic substitution at the carboxyl carbon, causing the cleavage of the ester bond and formation of diethatyl and its dechlorinated derivative, and at the amide carbon, yielding an ethyl ester derivative and its acid.These pathways also suggest that hydrolysis of diethatyl-ethyl was catalyzed by adsorption on the clay surface.     

TiO2/ZSM-5m光催化耦合过硫酸盐降解焦化尾水的研究

以具有介孔结构的沸石分子筛ZSM-5m负载纳米TiO2制备出复合型光催化剂,用扫描电镜、比表面及孔径分析仪和X射线衍射对形貌和结构进行表征,通过序批试验考察了TiO2/ZSM-5m/过硫酸盐体系深度降解焦化生化处理出水中残余有机污染物(ROPs)的效果和机理.结果表明,在COD初始平均浓度为352mg/L,TiO2/ ZSM-5m投加量为1.6g/L,pH值为3.0,C(Na2S2O8)为0.8g/L,常温下反应180min,COD出水平均浓度为76.3mg/L,去除率达到78.2 %,在上述优化条件下可达到现行污染物排放标准.ROPs光催化符合Langmuir-Hinshelwood模型,推测具有微介双孔结构的催化剂表面电子易被S2O82-俘获,降低空穴与电子的复合率,促进了·OH 和SO4-·形成,对ROPs的吸附和光降解有较大的强化作用.用GC-MS对处理前后废水中的污染物进行测定以揭示降解与转化规律,发现苯类特征污染物能有效降解,但产生的中间产物明显增多.     

Kinetics of selective catalytic reduction of NO by NH_3 on Fe-Mo/ZSM-5 catalyst

The catalyst of Fe-Mo/ZSM-5 has been found to be more active than Fe-ZSM-5 and Mo/ZSM-5 separately for selective catalytic reduction (SCR) of nitric oxide (NO) with NH_3.The kinetics of the SCR reaction in the presence of O_2 was studied in this work.The results showed that the observed reaction orders were 0.74-0.99,0.01-0.13,and 0 for NO,O_2 and NH_3 at 350-450℃,respectively. And the apparent activation energy of the SCR was 65 kJ/mol on the Fe-Mo/ZSM-5 catalyst.The SCR mechanism was also deduced. Adsorbed NO species can react directly with adsorbed ammonia species on the active sites to form N_2 and H_2O.Gaseous O_2 might serve as a reoxidizing agent for the active sites that have undergone reduction in the SCR process.It is also important to note that a certain amount of NO was decomposed directly over the Fe-Mo/ZSM-5 catalyst in the absence of NH_3.     

选择性催化还原NOx的V2O5/TiO2催化剂特性研究

采用浸渍法制备了V2 O5/TiO2 催化剂 ,研究了浸渍液和催化剂的红外光谱。利用XRD研究了催化剂中V2 O5的含量和晶相情况 ,V2 O5在催化剂载体表面呈单层分布 ,单层分布实验阈值为 7% ;利用程序升温 (TPD)法研究了NH3在催化剂表面上的脱附 ,起峰温度为40 9K ,峰顶温度为 487K ,出现一个化学脱附峰     

Kinetics of selective catalytic reduction of NO by NH3 on Fe-Mo/ZSM-5 catalyst

The catalyst of Fe-Mo/ZSM-5 has been found to be more active than Fe-ZSM-5 and Mo/ZSM-5 separately for selective catalytic reduction (SCR) of nitric oxide (NO) with NH3. The kinetics of the SCR reaction in the presence of O2 was studied in this work. The results show that the observed reaction orders were 0.74-0.99, 0.01-0.13, and 0 for NO, O2 and NH3, respectively, at 350-450℃. And the apparent activation energy of the SCR was 65 kJ/mol on the Fe-Mo/ZSM-5 catalyst. The SCR mechanism was also deduced. Adsorbed NO species can react directly with adsorbed ammonia species on the active sites to form N2 and H2O. Gaseous O2 might serve as a reoxidizing agent for the active sites that have undergone reduction in the SCR process. It is also important to note that a certain amount of NO was decomposed directly over the Fe-Mo/ZSM-5 catalyst in the absence of NH3.     

纳米Fe3O4负载的浮游球衣菌去除重金属离子的工艺研究

以纳米Fe₃O₄负载浮游球衣菌（Sphaerotilus natans）制备复合生物吸附剂,对此吸附剂进行表征并考察了其吸附水中重金属离子的性能.红外光谱分析表明,此复合生物吸附剂表面的主要活性基团为酰胺基（—CONH—）和羟基（—OH）.吸附性能研究表明,菌含量和流量是影响复合生物吸附剂吸附重金属离子的主要因素,在Cu²⁺初始浓度c₀<20 mg/L,菌含量1.5 g/L（菌/ Fe₃O₄＝3∶2）,流量0.96 L/h 时吸附剂对Cu²⁺的吸附效果最好;用稀盐酸对复合生物吸附剂进行再生,吸附剂可重复使用10次以上,再生液可重复使用3次; 吸附选择性为：Pb²⁺ > Cu²⁺ > Zn²⁺>Cd²⁺.     

不同金属改性的蒙脱土对普萘洛尔的吸附

采用浸渍法将蒙脱土用5种金属阳离子饱和,分别得到铁基蒙脱土、铜基蒙脱土、钾基蒙脱土、钠基蒙脱土和钙基蒙脱土,研究普萘洛尔在这5种金属阳离子饱和的蒙脱土上的吸附行为,探明主要影响因素,并推测可能的吸附机制。结果表明:5种金属阳离子饱和的蒙脱土对普萘洛尔均具有较高的吸附能力,且吸附能力顺序为铁基蒙脱土>铜基蒙脱土>钾基蒙脱土>钠基蒙脱土>钙基蒙脱土。pH为3~9时吸附量增加,是由于溶液中H+与普萘洛尔在金属阳离子饱和蒙脱土上吸附位点竞争力减弱;pH为9~11时吸附量减少,是由于普萘洛尔主要以分子状态存在,静电引力下降。K+、Na+和Ca2+的存在会抑制普萘洛尔的吸附。腐植酸加入会促进普萘洛尔的吸附,但促进作用随腐植酸浓度升高而减弱,甚至出现抑制作用。Langmuir等温吸附模型和准二级动力学方程能较好地描述普萘洛尔的吸附过程。研究结果有望为全面掌握普萘洛尔在土壤环境中的迁移转化规律提供的理论依据。     

Adsorption and desorption of SO2, NO and chlorobenzene on activated carbon

Activated carbon (AC) is very effective for multi-pollutant removal; however, the complicated components in flue gas can influence each other''s adsorption. A series of adsorption experiments for multicomponents, including SO₂, NO, chlorobenzene and H₂O, on AC were performed in a fixed-bed reactor. For single-component adsorption, the adsorption amount for chlorobenzene was larger than for SO₂ and NO on the AC. In the multi-component atmosphere, the adsorption amount decreased by 27.6% for chlorobenzene and decreased by 95.6% for NO, whereas it increased by a factor of two for SO₂, demonstrating that a complex atmosphere is unfavorable for chlorobenzene adsorption and inhibits NO adsorption. In contrast, it is very beneficial for SO₂ adsorption. The temperature-programmed desorption (TPD) results indicated that the binding strength between the gas adsorbates and the AC follows the order of SO₂ > chlorobenzene > NO. The adsorption amount is independent of the binding strength. The presence of H₂O enhanced the component effects, while it weakened the binding force between the gas adsorbates and the AC. AC oxygen functional groups were analyzed using TPD and X-ray photoelectron spectroscopy (XPS) measurements. The results reveal the reason why the chlorobenzene adsorption is less affected by the presence of other components. Lactone groups partly transform into carbonyl and quinone groups after chlorobenzene desorption. The chlorobenzene adsorption increases the number of C = O groups, which explains the positive effect of chlorobenzene on SO₂ adsorption and the strong NO adsorption.     

两种不同硅铝比的ZSM-5型分子筛去除水中Pb~(2+)的研究

考察硅铝比不同的ZSM-5两种分子筛(25H和50H,25和50为硅铝比:SiO2/Al2O3)对水中Pb2+离子的吸附去除效能。两种材料均可有效吸附去除水中Pb2+离子,吸附等温线符合Langmuir吸附等温式,25H的最大吸附容量达22.22mg/g,吸附动力学符合假二阶动力学模型,吸附速率及吸附容量顺序为:25H>50H。随着投加量的增加,分子筛对Pb2+的去除率呈上升趋势。常见共存阳离子均对分子筛吸附去除Pb2+产生影响。     

几种天然多孔矿物对钾肥的吸附及缓释效果

以KCl为钾源、斜发沸石、膨润土和凹凸棒石粘土3种天然多孔矿物为缓释载体,进行矿物对钾肥的吸附性能和缓释效果研究。探讨了吸附时间、K+初始浓度与吸附量的关系,确定出K+吸附量最大时的K+初始浓度。用pH=5的HCl溶液和(Ca2++Mg2+)浓度为1.6、3.2、6.4、12.8、19.2、25.6 mmol/L的混合溶液对各矿物缓释肥进行解吸。结果表明:各矿物对K+的吸附在30 min内达到平衡。斜发沸石、膨润土和凹凸棒石粘土对K+的饱和吸附量分别为44.53 mg/g、21.38 mg/g和13.97 mg/g。斜发沸石和膨润土对K+的吸附曲线符合Langmuir吸附等温式,凹凸棒石粘土对K+的吸附曲线总体符合Freundlich等温式。pH=5的HCl溶液对K+的解吸量最小,随解吸溶液中(Ca2++Mg2+)浓度增加,解吸量增大,解吸速率远小于吸附速率。斜发沸石的固钾能力最强,凹凸棒石粘土次之,膨润土相对最弱。     

Effects of bile salts and divalent cations on the adsorption of norfloxacin by agricultural soils

The effects of bile salts （sodium cholate and sodium deoxycholate, 0-20 mmol/L）, divalent cations （Ca^2＋, Mg^2＋, Cu^2＋ and Zn^2＋, 0-20 mmol/L） or pH （3.0-10.0） on the adsorption of norfloxacin by three selected soils （Paddy_H, Paddy_G and Red_J） were systematically studied. Soil adsorption of norfloxacin follows a pseudo second-order kinetics model, and the maximum adsorption capacity has been determined from the nonlinear fit of the Langmuir isotherm model to be 88.8, 88.1 and 63.0 μmol/g for the adsorption onto Paddy_H, Paddy_G and Red_J, respectively. The results indicate that norfloxacin has a high adsorption affinity for the agricultural soils tested and that the organic content of these soils have at least a slight influence on this adsorption. The adsorption of norfloxacin to soils was strongly dependent on pH and exhibited a maximum at approximately pH 6. The presence of divalent cations prominently suppressed the adsorption of norfloxacin by paddy soils, which followed an order of Cu^2＋ 〉 Mg^2＋ 〉 Ca^2＋ 〉 Zn^2＋, and by red soil, which followed an order of Cu^2＋ 〉 Zn^2＋ 〉 Ca^2＋ 〉 Mg^2＋. The adsorption of norfloxacin （by the soils studied） sharply decreased as the amount of bile salts was increased. For uncharged norfloxacin at environmentally relevant pH values, such factors as soil type, exogenous divalent cations and macromolecules significantly altered the environmental fate and transport of norfloxacin between aquatic and soil interfaces.     

基于灰度的生物炭pH值与N和K离子吸附研究

通过固定床石英管热解装置将稻壳、木薯秸秆及玉米秸秆在350、450、500、550、600℃进行充分热解制备生物炭,利用图像识别技术获得生物炭的RGB值（红、绿、蓝三个通道的颜色）及相应的灰度值,研究了生物炭灰度值与其水溶液中的pH值及阳离子（NH₄⁺-N及K⁺-K）吸附性能的关系.结果表明：3种生物炭的pH值随着灰度值的增加呈现“S”型增长趋势,并符合DoseResp模型,回归方程的决定系数（R²）分别为0.9766、0.9592和0.9219,残差平方和（RSS）均小于0.01;除玉米秸秆炭的K⁺-K吸附量与灰度值的关系为线性负相关外,3种生物炭的NH₄⁺-N和K⁺-K吸附量与灰度值之间满足一元高次非线性模型,R²范围在0.8595~0.9999.本研究为快速预测生物炭在水溶液中的pH值和阳离子吸附性能提供了理论基础.     

表面酸碱2步改性对活性炭吸附Cr(Ⅵ)的影响

研究了酸碱2步改性对活性炭吸附水相中Cr(Ⅵ)的影响.将活性炭(AC₀)在HNO₃溶液中氧化(AC₁),然后在NaOH和NaCl的混合液中处理(AC₂).分别采用平衡和连续吸附试验,测试Cr(Ⅵ)的吸附特征.以Boemh滴定法定量检测活性炭表面酸性官能团数量,结合元素分析结果定量表征活性炭的表面含氧官能团变化;以低温液氮(N₂/77K)吸附法分析活性炭的比表面积和孔径结构.结果表明:活性炭经2步改性后,其Cr(Ⅵ)的吸附容量和吸附速度均显著改变.吸附容量和吸附速度大小依次为AC₂>AC₁>AC₀.改性活性炭表面积下降,表面含氧酸性官能团数量增加.HNO₃液相氧化处理可使活性炭表面生成带正电含氧酸性官能团,第2步改性后活性炭表面酸性官能团H⁺部分被Na⁺取代,使活性炭表面酸性降低.表面较多的含氧酸性官能团(与AC₀相比)、适宜的表面pH(与AC₁相比)是AC₂所表现出较高Cr(Ⅵ)吸附容量的主要原因.     

沟戈登氏菌对重金属的生物吸附-浮选和解吸性能

用沟戈登氏菌作吸附剂,研究了采用生物吸附-浮选和解吸法从水溶液中去除和回收重金属的过程,并对生物吸附浮选机理进行了分析.结果表明,沟戈登氏菌对各种重金属离子的选择性为Hg>Pb>Cu,但菌细胞对Cu的吸附能力最高.NH₄⁺的加入对吸附Pb²⁺有促进作用,而K⁺、Na⁺、Ca²⁺和Mg²⁺共存离子的加入会对吸附过程有明显的抑制.当加入DA17.5mmol/L,pH为9.5时,Pb²⁺和菌细胞的去除率分别能够达到93%和96%,经无水Na₂CO3的₃次吸附、浮选和解吸处理后,它们的去除率仍然能够达到94%和97%.动电位和红外光谱分析结果表明,沟戈登氏菌的自然等电点为3.50,吸附Pb2+后增为4.02,与DA作用后降至3.02,吸附过程与细胞壁上的羧酸基团和乙酰胺基团有关,浮选过程则是有静电力、氢键、离子交换和化学络合等过程的协同作用.扫描电镜观察显示,吸附Hg²⁺后,菌细胞表明粘附有絮状物,菌体形状变得不规则.