活性焦负载MnO2对气态Hg0的吸附脱除研究

研究了活性焦(AC)及负载MnO2的活性焦(MnO2/AC)对气态Hg0的吸附脱除,发现负载MnO2到AC明显提高了其对Hg0的吸附脱除能力.考察了MnO2负载量、温度、Hg0浓度和烟气成分等对MnO2/AC吸附脱除Hg0的影响.结果表明,MnO2/AC对Hg0的吸附脱除能力随MnO2负载量的增加而增强;在120～200℃的温度范围内,随着温度升高,MnO2/AC对Hg0的吸附脱除能力增强;O2和HCl对MnO2/AC吸附脱除Hg0具有促进作用,而SO2和H2O具有抑制作用.SEM-EDX和逐级化学提取结果证实,MnO2将Hg0催化氧化为HgO并吸附在AC上,这是MnO2/AC具有较高的吸附脱除Hg0能力的原因.     

活性炭负载二氧化锰的制备及其对罗丹明B吸附效能

采用颗粒活性炭(GAC)以共沉淀和热分解法制备了改性活性炭(MnO_2-AC),并采用SEM、XRD表征手段对改性前后活性炭进行微观分析;进而研究了GAC和MnO_2-AC随染料初始浓度、活性碳投加量、温度、吸附时间变化对染料废水罗丹明B的吸附效果影响。结果表明:GAC经改性后,活性炭表面变得粗糙,并有MnO_2产生。在MnO_2-AC投加量为0.2 g,罗丹明B浓度为100 mg/L,温度为25℃条件下反应12 h,其吸附量达到36.80 mg/g。另外,MnO_2-AC对罗丹明B的吸附过程符合Langmuir等温模型,并遵循准二级动力学模型。     

V2O5/AC在含SO2气氛中对气态Hg0的吸附脱除研究

利用固定床反应器研究了模拟烟气(N_2、SO_2、O_2)气氛下,气态Hg~0在V_2O_5/AC催化剂上的吸附脱除行为.考察了V_2O_5担载量、SO_2浓度和吸附温度等对V_2O_5/AC吸附脱除Hg~0的影响,并对V_2O_5/AC上吸附汞的形态进行了XPS分析表征.研究发现,V_2O_5/AC对Hg~0的吸附能力远大于载体AC.汞的吸附量与V_2O_5/AC中V_2O_5的质量分数有关,随着V_2O_5质量分数从0.5%增加到1.0%,汞的吸附量从75.9 μg·g~(-1)增加到89.6 μg·g~(-1) (无氧) 和115.9 μg·g~(-1)增加到185.5 μg·g~(-1) (有氧),远高于相同吸附条件下的AC上的汞吸附量 (9.6 μg·g~(-1)和23.3 μg·g~(-1)).SO_2对Hg~0的吸附有促进作用,主要是由于SO_2和Hg~0在V_2O_5/AC上发生了化学反应.但是当SO_2体积分数从500×10~(-6)增加到2 000×10~(-6)时,V_2O_5/AC对汞的吸附量只增加了5%.不同温度下的实验结果表明,V_2O_5/AC催化剂在150℃左右的吸附脱除Hg~0的能力最高,汞的吸附量达到98.5 μg·g~(-1) (无氧) 和187.7 μg·g~(-1) (有氧).XPS 分析结果表明,在V_2O_5/AC催化剂表面有HgO和HgSO_4生成,证实了V_2O_5和SO_2的作用.     

Metal chlorides loaded on activated carbon to capture elemental mercury

Activated carbon (AC) was considered to be an effective sorbent to control mercury in combustion systems. However, its capture capacity was low and it required a high carbon-to-mercury mass ratio. AC loaded with catalyst showed a high elemental mercury (Hg0) capture capacity due to large surface area of AC and high oxidization ability of catalyst. In this study, several metal chlorides and metal oxides were used to promote the sorption capacity of AC. As a result, metal chlorides were better than metal oxides loaded on AC to remove gaseous mercury. X-ray diffractometer (XRD), thermogravimetric analyzer (TGA) and specific surface area by Brunauer- Emmett-Teller method (BET) analysis showed the main mechanisms: first, AC had an enormous surface area for loading enough MClx; second, Cl and MxOy were generated during pyrogenation of MClx; finally, there were lots of active elements such as Cl and MxOy which could react with elemental mercury and convert it to mercury oxide and mercury chloride. The HgO and HgCl2 might be released from AC’s porous structure by thermo regeneration. A catalytic chemisorption mechanism predominates the sorption process of elemental mercury. As Co and Mn were valence variable metal elements, their catalytic effect on Hg0 oxidization may accelerate both oxidation and halogenation of Hg0. The sorbents loaded with metal chlorides possessed a synergistic function of catalytic effect of valence variable metal and chlorine oxidation.     

Influence of moderate pre-oxidation treatment on the physical, chemical and phosphate adsorption properties of iron-containing activated carbon

A novel adsorbent based on iron oxide dispersed over activated carbon(AC) were prepared, and used for phosphate removal from aqueous solutions. The influence of pre-oxidation treatment on the physical, chemical and phosphate adsorption properties of iron-containing AC were determined. Two series of ACs, non-oxidized and oxidized carbon modified by iron(denoted as AC-Fe and AC/OFe), resulted in a maximum impregnated iron of 4.03% and 7.56%, respectively. AC/O-Fe showed 34.0%–46.6% higher phosphate removal efficiency than the AC-Fe did. This was first attributed to the moderate pre-oxidation of raw AC by nitric acid, achieved by dosing Fe(II) after a pre-oxidation, to obtain higher iron loading, which is favorable for phosphate adsorption. Additionally, the in-situ formed active site on the surface of carbon, which was derived from the oxidation of Fe(II) by nitric acid dominated the remarkably high efficiency with respect to the removal of phosphate. The activation energy for adsorption was calculated to be 10.53 and 18.88 kJ/mol for AC-Fe and AC/OFe, respectively. The results showed that the surface mass transfer and intra-particle diffusion were simultaneously occurring during the process and contribute to the adsorption mechanism.     

活性炭孔结构和表面化学性质对吸附硝基苯的影响

通过对活性炭HNO3氧化及随后的N2:气氛中热处理,研究了活性炭性质对其吸附硝基苯性能的影响.以低温液氮(N2/77K)吸附测定活性炭的比表面积和孔容、孔径分布,以SEM观测活性炭表面形貌,以Boehm滴定、FTIR、零电荷点pHpzc测定及元素分析定量表征活性炭表面含氧官能团变化.结果表明, HNO3氧化可以显著改变活性炭表面化学性质,增加活性炭表面酸性含氧官能团数量,对活性炭孔隙结构影响不大.随后N2:气氛中热处理可以造成活性炭表面酸性含氧官能团分解,外表面积增大,微孔烧蚀为中孔.硝基苯在活性炭上的吸附基本符合Langmuir方程,改性后活性炭对硝基苯的吸附容量明显改变, ACNO-T、ACraw、ACNO吸附容量分别为1011.31、483.09、321.54 mg·g-1.较大的外表面积、适宜数量的中孔以及较少的酸性含氧官能团是ACNO-T对硝基苯表现出较高吸附容量的主要原因.     

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.     

微波辐照制备花生壳活性炭研究

以花生壳为原料通过微波辐照制备了具有高比表面积并含有大量中孔的活性炭。讨论了活化剂类型、浸渍时间、浸渍比、活化剂浓度、微波功率和辐照时间对花生壳活性炭制备的影响。结果表明:相较磷酸和氢氧化钠,采用氯化锌活化剂制备的花生壳活性炭有更好的碘吸附性能;在浸渍浓度为40%,浸渍比为1∶6,浸渍时间为48 h,微波功率为500 W,辐照时间为6 min的条件下,制备的花生壳活性炭碘吸附值和亚甲基蓝吸附值分别为(898.6±12.8)mg/g和(46.2±3.8)mg/g;微波辐照工艺制备的活性炭,其碘吸附与亚甲基蓝吸附能力均优于马弗炉工艺;花生壳活性炭的碘吸附与亚甲基蓝吸附能力均优于市售活性炭。     

Formation of sulfur oxide groups by SO2 and their roles in mercury adsorption on carbon-based materials

The presence of SO₂ display significant effect on the mercury (Hg) adsorption ability of carbon-based sorbent. Yet the adsorption and oxidation of SO₂ on carbon with oxygen group, as well as the roles of different sulfur oxide groups in Hg adsorption have heretofore been unclear. The formation of sulfur oxide groups by SO₂ and their effects on Hg adsorption on carbon was detailed examined by the density functional theory. The results show that SO₂ can be oxidized into SO₃ by oxygen group on carbon surface. Both C-SO₂ and C-SO₃ can improve Hg adsorption on carbon site, while the promotive effect of C-SO₂ is stronger than C-SO₃. Electron density difference analyses reveal that sulfur oxide groups enhance the charge transfer ability of surface unsaturated carbon atom, thereby improving Hg adsorption. The experimental results confirm that surface active groups formed by SO₂ adsorption is more active for Hg adsorption than the groups generated by SO₃.     

汞在腐殖酸上的吸附与解吸特征

采用间歇法研究了汞在腐殖酸两组分（富里酸FA、胡敏酸HA）上的吸附－解吸量和动力学特征以及介质pH的影响，结果表明,腐殖酸对汞的吸附容量以FA＞HA，吸附强度以HA＞FA，从而使得解吸量以FA－Hg＞HA－Hg，腐殖酸与汞的吸附和解吸动力学，用Evolich方程描述最佳，且FA对汞的吸附速率和解吸速率都高于HA，在pH15．5以下，介质pH的升高利于腐殖酸更快地吸附更大量的汞，咀更难以解吸。     

FeCl3改性钢渣脱除燃煤烟气中Hg0的研究

以钢铁厂废弃钢渣为原料,以丙酮溶液为分散剂制备FeCl₃改性材料,在固定床吸附评价装置上考察了钢渣在FeCl₃改性前后对模拟烟气中Hg脱除效果的影响,并结合吸附试验与微观表征对改性催化剂的脱汞性能进行分析.结果表明:氯是FeCl₃改性钢渣吸附剂的主要活性组分,FeCl₃的掺入使钢渣的比表面积由1.06 m2/g提高到1.32 m2/g,进而提高吸附剂的汞吸附容量,经FeCl₃改性后废弃钢渣对汞的脱除效率比未改性前提升了3.2倍.SO₂的存在降低了FeCl₃改性钢渣材料的脱汞性能,持续通入的SO₂与吸附剂接触占据了部分孔道和表面活性位点,使得对单质汞的吸附效率下降,200℃时含有SO₂时的FeCl₃改性钢渣吸附剂吸附量比未通入SO₂气体的改性材料降低了75.57%;在含有HCl气体的烟气体系中,FeCl₃改性钢渣材料对汞的脱除效率从3432.70 ng/g升至10341.10 ng/g,并且随着反应温度的升高零价汞向氧化态汞转化的效率增加.研究显示,SO₂的存在降低了FeCl₃改性钢渣吸附剂的脱汞性能,而HCl气体有效地促进了FeCl₃改性钢渣吸附剂对零价汞（Hg0）的脱除.      

酸碱改性活性炭及其对甲苯吸附的影响

分别用酸溶液(H_2SO_4、HNO_3、H_3PO_4)和碱溶液(NaOH或NH_3·H_2O)浸渍方法对活性炭进行改性,并对酸改性活性炭进行碱溶液二次改性处理,通过表征改性前后活性炭BET比表面积、孔结构、表面官能团等理化特征和测定其对甲苯蒸气的饱和吸附量,研究了影响活性炭吸附甲苯蒸气的关键因素.结果表明,酸改性使BET比表面积、微孔面积、微孔容积减少、表面酸性官能团增加,而碱改性呈现相反的理化特征变化.活性炭理化特征的变化可能与改性溶液的酸碱性、氧化还原性有关,并且这种相反的变化直接关系到活性炭对甲苯蒸气的吸附.3种酸改性的活性炭对甲苯蒸气饱和吸附量相对于原活性炭减少9.6%~20.0%,而两种碱改性的活性炭则增加29.2%~39.2%.相关性分析显示甲苯吸附量与BET比表面积、微孔面积、微孔容积正相关,而与表面酸性官能团负相关;多元回归分析进一步表明微孔容积和酸性官能团数量是影响活性炭甲苯吸附的关键因素.二次改性活性炭甲苯吸附量与表面含氧酸性官能团拟合结果则表明,—COOH、C＝O和—OH都对活性炭甲苯吸附能力有影响,其中—COOH影响较大.研究结果表明有效提高活性炭对甲苯吸附能力,改性宜以提高活性炭微孔容积和减小活性炭表面酸性官能团数量,特别是—COOH数量为目标导向.     

腐殖酸对土壤吸持汞的影响研究

采用吸附 解吸热力学和动力学方法研究了腐殖酸各组份对土壤吸持汞的影响 ,发现该试验条件下 ,腐殖酸能提高土壤对汞吸持能力 ,但不同组份其作用效果不同 ,富里酸在提高土壤吸持汞方面作用较短暂且不稳定 ,胡敏酸在增强土壤吸附固定汞的数量和速率上却好于富里酸。     

Mercury removal from coal combustion flue gas by modified fly ash

Fly ash is a potential alternative to activated carbon for mercury adsorption. The effects of physicochemical properties on the mercury adsorption performance of three fly ash samples were investigated. X-ray fluorescence spectroscopy, X-ray photoelectron spectroscopy, and other methods were used to characterize the samples. Results indicate that mercury adsorption on fly ash is primarily physisorption and chemisorption. High specific surface areas and small pore diameters are beneficial to efficient mercury removal. Incompletely burned carbon is also an important factor for the improvement of mercury removal efficiency, in particular. The C-M bond, which is formed by the reaction of C and Ti, Si and other elements, may improve mercury oxidation. The samples modified with CuBr2 , CuCl 2 and FeCl3 showed excellent performance for Hg removal, because the chlorine in metal chlorides acts as an oxidant that promotes the conversion of elemental mercury (Hg0) into its oxidized form (Hg2+). Cu2+ and Fe3+ can also promote Hg 0 oxidation as catalysts. HCl and O2 promote the adsorption of Hg by modified fly ash, whereas SO2 inhibits the Hg adsorption because of competitive adsorption for active sites. Fly ash samples modified with CuBr2 , CuCl2 and FeCl3 are therefore promising materials for controlling mercury emissions.     

燃煤飞灰对锅炉烟道气中Hg0的吸附特性

在实验室模拟研究了燃煤飞灰颗粒组分对燃煤烟道气中气相Hg的吸附脱除特性.试验结果表明,Hg吸附量随飞灰烧失量的增长而增大,飞灰中不同类型介质的气相Hg吸附特性差异显著,其中未燃尽炭的Hg吸附性能最强,吸附剂BET比表面积与其Hg吸附量呈正相关关系.载气气相Hg浓度与Hg吸附量成非线性正相关关系,即Hg浓度为5×10^-7时的Hg吸附量只有5×10^-6的1/2.吸附温度与Hg吸附量呈较显著负相关关系.残炭表面的含氧官能团C=O有利于Hg的氧化和化学吸附.燃煤飞灰炭粒所具有的多孔隙结构和巨大比表面积有利于吸附脱除烟道气中Hg污染物.     

活性炭粒径对O3-AC处理有机废水的影响机制

臭氧-活性炭(O₃-AC)技术可以通过吸附和氧化协同作用去除废水中的污染物,而AC粒径是影响这一过程的关键因素。制备了5种48~1700 μm的不同粒径AC用于苯酚废水的O₃-AC处理,通过吸附和氧化动力学考察了AC粒径对污染物的吸附、氧化以及O₃传质的影响机制。结果表明:在AC粒径<150 μm时,AC表面出现更多微观孔道,吸附和氧化速率较粒径>150 μm的AC分别提高了189%和166%;粒径在48~150 μm的AC在O₃中的传质和分解速率分别达到0.57,0.51 min-1,显著高于其他大粒径AC;在O₃-AC中加入叔丁醇(TBA)后,40 min内COD去除率降低了20%,O₃的分解作用与催化氧化反应有关;使用48~150 μm粒径的AC连续进行6次O₃-AC实验,COD去除速率均保持在95%以上,具有良好稳定性。     

新型胺化介孔炭的制备及其对Pb(II)的吸附

采用微波辅助磷酸活化制备了高中孔率蔗渣基介孔炭,并通过硝酸氧化和乙二胺聚合在其孔道内修饰了含氮多胺基团,探索了溶液浓度、温度、吸附剂剂量等对改性介孔炭的Pb(II)吸附性能、行为和热力学特性的影响.结果表明,蔗渣基介孔炭较宽的孔道结构可通过乙二胺缩水聚合反应在其表面接枝酰胺、仲胺等含氮基团;胺化改性增强化了介孔炭对水溶液中Pb(II)的固定作用,改性后介孔炭对Pb(II)的吸附量高达180mg/g,是改性前介孔炭的1.5倍;改性介孔炭对Pb(II)的去除率显著增加,对溶液浓度<60mg/L的Pb(II)去除率接近100%.等温吸附与热力学数据表明,胺化改性介孔炭对Pb(II)的吸附位能量存在差异化,吸附是自发的吸热反应过程,温度对铅(II)离子吸附有促进作用,化学作用在吸附过程中发挥了重要作用.     

Activated carbons derived from oil palm empty-fruit bunches： Application to environmental problems

Activated carbons derived from oil palm empty fruit bunches （EFB） were investigated to find the suitability of its application for removal of phenol in aqueous solution through adsorption process, Two types of activation namely; thermal activation at 300, 500 and 800℃and physical activation at 150℃ （boiling treatment） were used for the production of the activated carbons. A control （untreated EFB） was used to compare the adsorption capacity of the activated carbons produced from these processes. The results indicated that the activated carbon derived at the temperature of 800℃ showed maximum absorption capacity in the aqueous solution of phenol. Batch adsorption studies showed an equilibrium time of 6 h for the activated carbon at 800℃. It was observed that the adsorption capacity was higher at lower values of pH （2-3） and higher value of initial concentration of phenol （200-300 mg/L）. The equilibrium data fitted better with the Freundlich adsorption isotherm compared to the Langmuir. Kinetic studies of phenol adsorption onto activated carbons were also studied to evaluate the adsorption rate. The estimated cost for production of activated carbon from EFB was shown in lower price （USD 0.50/kg of activated carbon） compared the activated carbon from other sources and processes.     

Vapor-phase elemental mercury adsorption by residual carbon separated from fly ash

Introduction The impact of mercury on the environment and thephysiological health of human is well documented(Laudal,2000; Poissant, 2002; Galbreath, 2000; Palusova, 1991).Mercury, especially methyl mercury, has high affinities forfatty tissue…     

硫改性牛粪生物炭对Hg2+的高效吸附及其机理

以牛粪为原料在400,500,600 ℃条件下限氧热解制备牛粪生物炭(BC),然后以不同质量比将升华硫和BC混合共热解制备硫改性牛粪生物炭(BCS)。使用元素分析仪、SEM、FTIR、XPS和BET对制得的BC和BCS进行了表征,并研究了各BC和BCS对Hg2+的吸附特性。结果表明:热解过程使BC和BCS变得粗糙多孔,Hg2+被吸附到生物炭表面和孔道内;BC和BCS的吸附过程符合准二级动力学模型,BCS对Hg2+的吸附平衡时间仅为30 min,且吸附过程不受pH影响;Langmuir模型可较好地描述BC吸附过程,吸附量随热解温度的升高而降低,BCS吸附过程符合Freundlich模型,吸附能力较BC显著提升,最大拟合吸附量达到407.81 mg/g;BCS的吸附稳定性较高,在各解吸剂中的解吸率均低于5%;BC主要吸附机理为官能团络合,BCS主要吸附机理为HgS沉淀。因此BCS是一种高效稳定的Hg2+吸附材料。