不同结构水钠锰矿催化氧化对苯二酚腐殖化程度的差异及其原因分析

本文合成了一系列不同氧化度的酸性和碱性水钠锰矿,以对苯二酚作为腐殖质形成的前驱物,分析水钠锰矿矿物类型和亚结构变化对对苯二酚腐殖化程度的影响。取得的主要结果有:水钠锰矿的矿物类型和亚结构(锰氧化度、八面体空位、H+、Mn4+和Mn3+含量)对对苯二酚的腐殖化程度具有重要的影响,且矿物类型的影响大于同种矿物不同亚结构产生的影响。酸性水钠锰矿比碱性水钠锰矿含有更多的H+,导致酸性水钠锰矿比碱性水钠锰矿具有更高的氧化容量,反应达到平衡后,对苯二酚腐殖化程度更高。因此,水钠锰矿物中H+含量对对苯二酚腐殖化程度的影响要大于矿物中Mn4+和Mn3+含量的影响。同种类型水钠锰矿氧化度越高,得电子量将越多,氧化容量越大,反应达到平衡后,对苯二酚腐殖化程度越高。     

成熟锰砂表面细菌的分离及其氧化铁锰能力

从取自不同电厂成熟锰砂表面的活性滤膜中分离出7种细菌,经鉴定分别属于纤发菌属、球衣菌属、鞘铁细菌属.研究表明,这3个菌属的微生物对水中Fe2+都具有较好的去除效果,其中鞘铁细菌1号对铁的去除效果最好;纤发菌和鞘铁细菌对水中Mn2+都具有良好的去除效果,其中鞘铁细菌1号的去除能力最强,鞘铁细菌2号次之.将分别堵养的具有氧...     

负载型膨胀石墨催化剂低温催化氧化NO研究

膨胀石墨(EG)具有四级孔结构,是一种优良的吸附剂和催化剂载体.采用超声浸渍法制备了Mn/EG催化剂,用于低温催化氧化NO,考察了金属负载量、进口NO质量浓度及O2体积分数对NO氧化效率的影响.结果表明,利用超声浸渍法制备得到的Mn/EG催化剂低温催化氧化活性较好,且催化剂表面的3价Mn对反应活性有重要影响.进口气体中O2体积分数对反应活性有明显的影响,低温时高体积分数的氧能促进NO的转化.150℃时,在NO体积分数为0.05％、O2体积分数为3％、空速为47 770 h-1的条件下,该催化剂的NO催化氧化效率可达42％.     

A kinetic study of Mn(II) precipitation of leached aqueous solution from electrolytic manganese residues

Electrolytic manganese residue (EMR) is a type of solid waste discharged from the process that converts solid manganese carbonate of rhodochrosite into soluble Mn(II) and generates anode mud under electrolysis. The experimental material was a filtrate created by using distilled water as a dispersal agent for the EMR, followed by simple filtration. A calculated amount of sodium carbonate was added to recover the soluble Mn(II) via precipitation into manganese carbonate. Data showed that Mn concentration may be markedly decreased from 2069 to 36 mg/L, thereby reaching a recovery rate as high as 98%. Analysis demonstrated that precipitation of Mn(II) from a leached aqueous solution followed first-order kinetics. The findings indicate that the reaction rate constant decreased as temperature gradually rose and that its apparent activation energy E_a was ?10.48 kJ/mol.     

Abatement of SO2–NOx binary gas mixtures using a ferruginous active absorbent: Part I. Synergistic effects and mechanism

A novel ferruginous active absorbent, prepared by fly ash, industrial lime and the additive Fe(VI), was introduced for synchronous abatement of binary mixtures of SO₂–NOx from simulated coal-fired flue gas. The synergistic action of various factors on the absorption of SO₂ and NOx was investigated. The results show that a strong synergistic effect exists between Fe(VI) dose and reaction temperature for the desulfurization. It was observed that in the denitration process, the synergy of Fe(VI) dose and Ca/(S + N) had the most significant impact on the removal of NO, followed by the synergy of Fe(VI) and reaction temperature, and then the synergy of reaction temperature and flue gas humidity. A scanning electron microscope (SEM) and an accessory X-ray energy spectrometer (EDS) were used to observe the surface characteristics of the raw and spent absorbent as well as fly ash. A reaction mechanism was proposed based on chemical analysis of sulfur and nitrogen species concentrations in the spent absorbent. The Gibbs free energy, equilibrium constants and partial pressures of the SO₂–NOx binary system were determined by thermodynamics.     

固液界面NOM吸附中疏水效应的影响研究

文章以腐殖酸和纳米Fe2O3为对象,着重研究了腐殖酸分子在纳米Fe2O3表面的吸附过程中的疏水效应,借助红外光谱和热重等分析方法研究了腐殖酸吸附前后的疏水性随溶液环境变化的规律。结果表明,当离子强度为0、0.005、0.01和0.05 mol/kg,pH值从7变到12时,纳米Fe2O3吸附溶解性腐殖酸分子后形成的复合体的热失重量随着pH值的升高先减小后增大。当pH值从7升高到10时,亲水性降低,疏水性增强;当pH值从10升高到12时,亲水性增强,疏水性降低。当离子强度为0.001 mol/kg,pH值从7变到12时,复合体的热失重量随着pH值的升高而减小,亲水性降低,疏水性增强。当pH值为定值,离子强度变化时,纳米Fe2O3吸附溶解性腐殖酸分子后形成的复合体的热失重量随着离子强度的增加不断变化,曲线呈现出波动趋势,亲、疏水性在交替变化。红外光谱分析结果说明,对纳米Fe2O3吸附溶解性腐殖酸分子后形成的复合体的亲疏水性起主要影响的官能团可能是亲水性的羟基-OH、羰基C=O和疏水性的CH2烷烃。     

Cr(Ⅵ)在Fe(Ⅲ)-柠檬酸盐体系中紫外光还原研究

研究了在紫外光照射下,Fe(Ⅲ)-柠檬酸盐溶液对Cr(Ⅵ)的光还原反应.同时,考察了溶液pH值、Fe(Ⅲ)浓度、柠檬酸盐浓度、Cr(Ⅵ)初始浓度对光还原效率的影响,并分析了光还原反应的动力学.研究结果表明,Fe(Ⅲ)-柠檬酸盐体系能光还原Cr(Ⅵ),在pH为2.0～6.0的范围内,Cr(Ⅵ)的还原率随着溶液初始pH值的降低而增大.当pH值为2.0、Fe(Ⅲ)浓度为10μmol·L-1、柠檬酸盐浓度为250μmol·L-1及Cr(Ⅵ)初始浓度为19.2μmol·L-1时,光照反应8min后Cr(Ⅵ)的最大还原率达到100%,但当pH值增加到6.0时,Cr(Ⅵ)的最大还原率下降到19%;当Cr(Ⅵ)的初始浓度在9.6～96.0μmol·L-1的范围内时,Cr(Ⅵ)光还原反应的初始速率随着Fe(Ⅲ)、柠檬酸盐(cit3)、Cr(Ⅵ)初始-浓度的增加而增加.表观动力学方程为:-dCCr(Ⅵ)/dt=0.1019[Cr(Ⅵ)]0.[Fe(Ⅲ)]0.[cit3]0..536-25     

三江平原不同土地利用方式下土壤锰含量研究

通过对比分析三江平原典型的小叶章湿地、玉米地、水稻田、人工杨树林和岛状林土壤中锰（Mn）含量,研究了不同土地利用方式下土壤Mn分布特征及影响因素.结果表明,三江平原土壤Mn含量范围为107.73～2 798.99 mg.kg-1,平均为403.24 mg.kg-1,处于较低的水平.不同利用方式下土壤中Mn含量差异显著（F=9.272,P〈0.001）,表现出岛状林〉人工杨树林〉玉米地〉小叶章湿地〉水稻田的规律;总体上由表层至底层,各层土壤Mn含量表现为玉米地〉小叶章湿地〉水稻田,岛状林〉人工杨树林的规律,表明湿地开发为旱田后,土壤Mn将聚集,而开发为水田后,土壤Mn则流失.相关性分析表明,土壤中Mn含量与pH呈显著的负相关系（r=-0.279,P〈0.05）,Mn与S含量（r=0.383,P〈0.01）和可溶性有机碳含量（r=0.244,P〈0.05）呈显著的正相关关系,而与土壤有机质（SOM）和有效硫（Sa）含量相关性并不显著.环境因子的改变,可能是通过改变Mn的赋存状态而影响到土壤Mn含量.     

4,4’-二溴联苯在水溶液中光降解的动力学研究

多溴联苯作为溴代阻燃剂被广泛应用,从而广泛存在于环境。但少有对于多氯联苯环境行为的研究。文章以4,4’-二溴联苯为研究对象,模拟自然环境,探讨了光源强度、初始浓度、pH值和溶解氧等因素对4,4’-二溴联苯降解的影响,以及在模拟太阳光的照射下,研究了Fe3+和腐殖酸对4,4’-二溴联苯在水溶液中光降解速率的影响。结果表明,在高压汞灯照射下,4,4’-二溴联苯的光降解过程符合准一级动力学规律。提高光源强度可加速4,4’-二溴联苯的降解;初始浓度的增加使4,4’-二溴联苯降解速率减慢;反应液在高pH值和低pH值时,均促进4,4’-二溴联苯的光降解进程;体系中溶解氧增多也同样促进4,4’-二溴联苯的降解;小剂量的添加腐殖酸和Fe3+可以促进4,4’-二溴联苯的降解,但超过一定浓度则抑制其光降解。     

Catalytic dechlorination of o-cllorophenol by nanoscale Pd/Fe

Transformation of chlorophenols by nanoscale bimetallic particles represents one of the latest innovative technologies for environmental remediation. Nanoscale Pd/Fe bimetallic particles were synthesized in the laboratory for treatment of o-chlorophenol. Most of the nanoscale particles are in the size range of 20-100 nm. BET specific surface area of the nanoscale Pd/Fe particles is 12.4 m2/g. In comparison, a commercially available Fe powder( ＜100 mesh) has a specific surface area of just 0.49 m2/g. Batch experiments demonstrated that the nanoscale Pd/Fe bimetallic particles can effectively dechlorinate o-chlorophenol. Dechlorination efficiency is affected by the mass fraction of Pd in the bimetal, nanoscale Pd/Fe mass concentration and mixing intensity.