Enhanced activation of peroxymonosulfate by Fe/N co-doped ordered mesoporous carbon with dual active sites for efficient removal of m-cresol

The novel Fe-N co-doped ordered mesoporous carbon with high catalytic activity in m-cresol removal was prepared by urea-assisted impregnation and simple pyrolysis method.During the preparation of the Fe-NC catalyst,the complexation of N elements in urea could anchor Fe,and the formation of C3N4during urea pyrolysis could also prevent migration and aggregation of Fe species,which jointly improve the dispersion and stability of Fe.The FeN4sites and highly dispersed Fe nanoparticles synergistically trigger the dual-site peroxymonosulfate (PMS) activation for highly efficient m-cresol degradation,while the ordered mesoporous structure of the catalyst could improve the mass transfer rate of the catalytic process,which together promote catalytic degradation of m-cresol by PMS activation.Reactive oxygen species (ROS) analytic experiments demonstrate that the system degrades m-cresol by free radical pathway mainly based on SO_(4)^(-)·and·OH,and partially based on·OH as the active components,and a possible PMS activation mechanism by 5Fe-50 for m-cresol degradation was proposed.This study can provide theoretical guidance for the preparation of efficient and stable catalysts for the degradation of organic pollutants by activated PMS.

Dissimilatory reduction of Fe^III (EDTA) with microorganisms in the system of nitric oxide removal from the flue gas by metal chelate absorption

In the system of nitric oxide removal from the flue gas by metal chelate absorption, it is an obstacle that ferrous absorbents are easily oxidized by oxygen in the flue gas to ferric counterparts, which are not capable of binding NO. By adding iron metal or electrochemical method, Fe III (EDTA) can be reduced to Fe II (EDTA). However, there are various drawbacks associated with these techniques. The dissimilatory reduction of Fe III (EDTA) with microorganisms in the system of nitric oxide removal by metal chelate absorption was investigated. Ammonium salt instead of nitrate was used as the nitrogen source, as nitrates inhibited the reduction of Fe III due to the competition between the two electron acceptors. Supplemental glucose and lactate stimulated the formation of Fe II more than ethanol as the carbon sources. The microorganisms cultured at 50℃ were not very sensitive to the other experimental temperature, the reduction percentage of Fe III varied little with the temperature range of 30—50℃. Concentrated Na 2CO 3 solution was added to adjust the solution pH to an optimal pH range of 6—7 The overall results revealed that the dissimilatory ferric reducing microorganisms present in the mix culture are probably neutrophilic, moderately thermophilic Fe III reducers.

Fe(Ⅲ)对Anammox污泥脱氮效能长短期影响

通过接种厌氧氨氧化(Anammox)污泥,研究了Fe(Ⅲ)对Anammox污泥脱氮效能长短期影响.结果表明,适量提升Fe(Ⅲ)浓度可以提升Anammox菌的活性.当进水Fe(Ⅲ)浓度达到0.09mol/L时,反应器氮去除速率最高为0.238kg/(L·d),较对照组提升了14.2%.继续提高进水Fe(Ⅲ)浓度,氮去除速率逐步下降,当Fe(Ⅲ)浓度升至0.18mol/L时,氮去除速率降至0.215kg/(L·d),与最高氮去除速率相比下降10.75%.采用Haldane抑制动力学模型拟合得到Fe(Ⅲ)对Anammox半速率常数(KFe)为0.012mol/L,半抑制常数(KI)为0.449mol/L.长期结果表明,在0.09mol/L Fe(Ⅲ)浓度下,Anammox氮去除速率增幅最快,并且随着Fe(Ⅲ)浓度增加而逐步降低.由于Fe(Ⅲ)代替了NO_(2)^(-)-N作为电子受体发生厌氧铁氨氧化反应,在含有Fe(Ⅲ)的反应器中NO_(2)^(-)-N与NH_(4)^(+)-N的转化比在1.108~1.227之间波动,明显低于理论值1.32,并随Fe(Ⅲ)浓度的提升而降低.扫描电镜结果表明,添加Fe(Ⅲ)可使Anammox菌细胞结构更加稳定.

Fe(Ⅱ)对CANON工艺处理城镇污水脱氮性能的影响

全程自养脱氮(CANON)工艺,作为新型脱氮工艺应用于城镇污水深度脱氮过程中,有望降低污水处理的运行费用。考察了亚铁离子[Fe(Ⅱ)]对CANON工艺启动及稳定运行时脱氮性能的影响。结果表明:15~23℃条件下投加6.3 mg/L Fe(Ⅱ)时,可有效启动并稳定运行CANON工艺处理城镇污水,该工艺氮去除负荷(NRR)、总氮去除率(TNRE)和氨氮去除率(ARE)分别为(4.8±1.1)g-N/(L^(3)·d)、(97±1)%和(44.2±9.3)%;相关性分析表明,通过调控Fe(Ⅱ)投加量可有效抑制亚硝酸盐氧化菌(NOB)的活性;本次优化的Fe(Ⅱ)投加量为6.3 mg/L,其对CANON工艺脱氮性能的影响机制与CANON工艺中功能微生物活性的提高、Fe(Ⅱ)与进水氨氮及其他氮化合物的循环反应、铁型反硝化过程以及铁型厌氧氨氧化过程的耦合有关。

电化学系统内Feammox/NDFO耦合工艺脱氮效能和机理

针对目前Feammox/NDFO耦合工艺启动慢、脱氮效能不理想等缺陷,提出基于电化学原理强化Feammox/NDFO耦合工艺的策略.实验室内搭建生物电化学系统(BES)序批式厌氧反应器(B组),同时以不加电化学系统的普通厌氧反应器(A组)为对照组.A、B两组反应器共运行100d,分析了两反应器Feammox/NDFO耦合工艺启动过程中的脱氮效能、脱氮路径验证及种群结构组成,并探讨了BES系统Feammox/NDFO强化脱氮的机理.结果表明,实验组(B组)内NH_(4)^(+)-N去除率显著提高,第76d去除率趋于100%,TN去除率达65.83%;而对照组(A组)在第100d时,对NH_(4)^(+)-N和TN的去除率分别为50.22%和43.01%.脱氮路径验证实验结果表明,A、B组反应器内均有Feammox、NDFO、Anammox反应发生;并且B组反应器内反硝化速率明显大于A组.高通量测序结果表明,B组中铁循环脱氮功能菌中Desulfobacterota菌门的相对丰度较A组提高了2.34%;Thiobacillus和Denitratisoma丰度较A组分别提高了1.13%和0.87%.BES反应体系加速富集铁循环脱氮功能菌群,并可通过BES电极进行胞外电子转移,从而达到增强脱氮效能.

Efficient removal of Al(Ⅲ)and P507 from high concentration MgCl_(2)solution based on in-situ reaction strategy

For a highly efficient recycling of a wastewater containing a high concentration of MgCl_2,Al(Ⅲ)and P507 were scheduled to be removed in advance.In this study,the in-situ removal of Al(Ⅲ)and P507 from a high concentration MgCl_(2)solution at different pH values and Al/P molar ratios was investigated.The results showed that P507 formed organic complexes of Al_x(OH)_y~(Z+)-P507 at pH of 2.0-4.0.At pH of 4.0-5.0,Al(Ⅲ)precipitated and transferred into Al(OH)_(3)with a flocculent amorphous morphology.Active sites on the Al(OH)_(3)surface enhanced the removal efficiency of P507.At pH of 6.0-6.5,Al(Ⅲ)and Mg(Ⅱ)formed layered crystalline Al(OH)_(3)and MgAl_2(OH)_(8with)small pore channels and fewer active sites,resulting in a reduced removal efficiency of P507.When the Al/P molar ratio exceeded 13 and the pH was between 4.0 and 5.0,the removal rates of both Al(Ⅲ)and P507 were higher than98%,while the concentration loss of Mg(Ⅱ)was only 0.2%-0.9%.

Elimination, Kinetics and Thermodynamics of Fe(II) Ions by Adsorption in Static and Dynamic Conditions on Activated Carbons in Aqueous Media

This work investigated the removal, kinetics and thermodynamics of iron(II) ions (Fe(II)) by adsorption in static and dynamic conditions in aqueous media on activated carbons (AC-i30min, AC-i1h, and AC-i24h), prepared from palm nut shells collected in the city of Franceville to Gabon, using potassium hydroxide (KOH) as the activating agent. Results on the elimination of Fe(II) in static and dynamic adsorption on prepared activated carbons (ACs) showed that the AC-i24h adsorbent has the best Fe(II) adsorption capacities at saturation (Qsat). The Qsat obtained on AC-i24h in static and dynamic conditions (17.87 and 10.38 mg/g, respectively) were higher than those of AC-i30min (13.89 and 5.54 mg/g respectively) and AC-i1h (14.92 and 8.64 mg/g respectively). Moreover, the static adsorption was more effective in the removal of Fe(II) ions in aqueous media in our experimental conditions. The percentage removal (%E) of Fe(II) obtained on prepared activated carbons in static conditions was better than those obtained in dynamic conditions, especially on AC-i24h, where the %E was 89.27% in static and 61.56% in dynamic. In kinetics, results showed that the pseudo-second-order kinetic model best described the adsorption mechanisms of Fe(II) on prepared activated carbons in static adsorption, with mainly of chemisorption on the solid surfaces. However, in dynamic conditions, the pseudo-first-order kinetic model was more suitable. In addition to the weak interactions between Fe(II) and the activated carbon surfaces, strong interactions (chemisorption) were also observed. Also, thermodynamic data obtained on AC-i24h in static adsorption indicated that the adsorption of Fe(II) was spontaneous and increased with temperature (ΔG˚ H˚ = 503.54 KJ/mol).

基于六偏磷酸钠-Fe^(2+)的铁盐脱氮反应器运行性能及微生物学特征研究

以实验室高效反硝化反应器中的反硝化污泥作为接种污泥,启动自养型六偏磷酸钠-Fe^(2+)脱氮反应器,试验采用模拟废水通过88 d的不间断运行,研究了铁盐脱氮工艺的脱氮效能及其微生物学特性。结果表明,当反应器硝态氮容积负荷为0.42 kg/(m^(3)·d)时,最高稳定氮去除负荷为0.41 kg/(m^(3)·d);当Fe^(2+)容积负荷为4.92 kg/(m^(3)·d)时,最大铁去除负荷为2.77 kg/(m^(3)·d)。反应器稳定运行时硝态氮、Fe^(2+)的去除率分别达94.6%、52.6%,最佳效能可维持28 d。反应器运行到第82天时,颗粒污泥由黄色变为灰褐色,颗粒解体,污泥比活性逐渐升高,比反硝化活性由0.71 mg[N]/(g[VSS]·h)升高到2.3 mg[N]/(g[VSS]·h),同比上升224%;比铁氧化活性由7.3 mg[Fe]/(g[VSS]·h)升高到15 mg[Fe]/(g[VSS]·h),同比上升105%。六偏磷酸钠-Fe^(2+)脱氮作为一种新型自养反硝化技术,不仅增强了活细菌的生物活性和反硝化活性,还延长了铁盐脱氮污泥反硝化的高效期。

伯胺(N1923)-正辛烷在硫酸体系中萃取和反萃Fe(III)机理的研究

对伯胺—正辛烷萃取体系在萃取和反萃过程中有机相组成和水含量的变化用FTIR和光子相关谱进行分析研究。结果表明:伯胺与水相酸作用生成了阳离子型表面活性剂的结构,在有机相中易生成反相胶团。其萃取和反萃过程的实质是反相胶团内外的阳离子交换过程。Fe(Ⅲ)以水合形式萃取入有机相中,Fe(Ⅲ)的水解可能发生在反相胶团的微环境中。

水杨醛缩三乙烯四胺Schiff碱Fe(III)配合物的合成、结构和光谱性质

合成水杨醛缩三乙烯四胺Schiff碱Fe(Ⅲ)配合物[(saltrien)Fe]Cl.2H2O。采用元素分析、红外光谱、电子光谱对其结构进行了表征,晶体结构通过X-射线衍射法测定。该化合物的化学计量式为:20H29ClFeN4O4,晶体属单斜晶系,其空间群为P21/c。晶胞参数:a = 18.517(4), b = 9.985(2), c = 12.035(2) , b = 103.43(2)o, V = 2164.3(7) 3, Z = 4, F(000) = 1008, r = 1.475 g/cm3, Mr = 480.77, m (MoKa) = 0.855 cm-1。结构偏离因子R1 = 0.0345, wR2 = 0.0469。共收集到4566个独立衍射点,其中I>2 (I)的可观测点为3730个。

双水杨醛邻苯二胺与Fe(III)的显色反应研究及应用

研究了双水杨醛邻苯二胺(SALOPHEN)与Fe(III)的显色反应,试验表明,在pH=2.21的氨基乙酸-盐酸缓冲介质中,在阴离子表面活性剂十二烷基磺酸钠(SDS)存在下,Fe(III)与双水杨醛邻苯二胺(SALOPHEN)形成1:1稳定的棕色配合物。其最大吸收峰位于462nm处,表观摩尔吸光系数为4.1'104。铁浓度在0-4.5mg/ml范围内符合比尔定律。方法具有较高的灵敏度和选择性。应用于食品样品中微量铁的测定,结果满意。

Fe^(0)/C诱导铜盐还原耦合化学沉淀法脱除废水硫氰酸盐

焦化废水是一类伴随焦炭生产而形成的有机-无机组分共存、环境危害大的工业废水,其高含量的硫氰酸盐将毒害微生物、抑制生物活性,影响废水生化系统的稳定性,研究硫氰酸盐的资源化利用具有重要意义。采用等体积浸渍结合碳热还原法制备系列生物炭负载零价铁材料(Fe^(0)/C),用X射线衍射和氮气吸-脱附技术进行物性结构表征;模拟焦化废水,利用零价铁还原铜盐耦合硫氰酸亚铜合成反应,实现硫氰酸根回收利用。表征结果表明:Fe^(0)/C是无定形碳负载零价铁材料,比表面积较小(小于1 m^(2)/g)。实验结果显示,在模拟废水硫氰酸盐质量浓度为2.50 g/L、铜盐浓度为0.03 mol/L、pH为5.5、温度为40℃条件下反应10 min,3Fe^(0)/C(铁质量分数为3%)对硫氰酸盐脱除率达到99%,实现了模拟焦化废水中硫氰酸盐的高效脱除,获得了附加值较高的硫氰酸亚铜产品,丰富了焦化废水物化-生化处理技术理论。

Fabrication of Poly（y-glutamic acid）-coated Fe3O4 Magnetic Nanoparticles and Their Application in Heavy Metal Removal

In this study, poly（y-glutamic acid）-coated Fe3O4 magnetic nanoparticles （y-PGA/Fe304 MNPs） were successfully fabricated using the co-precipitation method. Fe3O4 MNPs were also prepared for comparison. The av erage size and specific surface area results reveal that 7-PGA/Fe304 MNPs （52.4 nm, 88.41 m2.g-1） have smaller particle size and larger specific surface area_ than Fe3O4 MNPs （62.0 nm, 76.83 mLg-1）. The y-PGA/Fe3O4 MNPs

High Efficient Removal of Trace Molybdenum from Water by FeCl_3:Effects of p H and Affecting Factors in the Presence of Co-existing Background Constituents

The effect of FeCl_3 coagulation-filtration on the removal of trace Mo(Ⅵ) from water is investigated in the p H range of 4. 00 to 9. 00 and the effects of sulfate,silicate,phosphate and humic acid( HA) on the process were determined. Overall,the removal of Mo(Ⅵ) is determined by two factors: the content of Fe intercepted from water( Intercepted Fe) and the affinity between Mo(Ⅵ)( or co-existing background constituents) and adsorption sites. At low p H,where the agglomeration of the iron flocs is limited,the former factor is dominant,so the methods that can promote the agglomeration of the iron flocs,such as increasing the p H,adding co-existing constituents( sulfate,phosphate or HA),can increase the removal of Mo(Ⅵ). While at high p H,the second factor dominated. Increasing the p H weakens the affinity between Mo(Ⅵ) and the iron flocs,and co-existing background constituents( sulfate,phosphate,silicate or HA) compete with Mo(Ⅵ) for adsorption sites,both effects result in a decrease in Mo(Ⅵ) removal. The Mo(Ⅵ) removal efficiency of FeCl_3 in natural water decreases as the p H increases from 4. 00 to 9. 00,and it is better to operate the coagulation process at p H 5.00 in the practical water treatment engineering.

Absorption performance of DMSA modified Fe_3O_4@SiO_2 core/shell magnetic nanocomposite for Pb^(2+) removal

The purpose of this study is to explore the adsorption performance of meso-2,3-dimercaptosuccinic acid(DMSA)modified Fe3O4@SiO2 magnetic nanocomposite(Fe3O4@SiO2@DMSA)for Pb2+ions removal from aqueous solutions.The effects of solution pH,initial concentration of Pb2+ions,contact time,and temperature on the amount of Pb2+adsorbed were investigated.Adsorption isotherms,adsorption kinetics,and thermodynamic analysis were also studied.The results showed that the maximum adsorption capacity of the Fe3O4@SiO2@DMSA composite is 50.5 mg/g at 298 K,which is higher than that of Fe3O4 and Fe3O4@SiO2 magnetic nanoparticles.The adsorption process agreed well with Langmuir adsorption isotherm models and pseudo second-order kinetics.The thermodynamic analysis revealed that the adsorption was spontaneous,endothermic and energetically driven in nature.

Removal of tungsten from molybdate solution by Fe-Mn binary oxide adsorbent

Considering the different geochemical enrichment behaviors of W and Mo,Fe?Mn binary oxide(FMBO),ferric hydroxide(Fe(OH)3)and manganese dioxide(MnO2)were studied to separate W from molybdate solution,respectively.The experimental results demonstrated that Fe?Mn binary oxide(FMBO)was the most suitable adsorbent for the separation.Under a wide pH(6.9?11.3)region,more than80%W removal efficiency and less than3%Mo loss could be obtained.In addition,the Fe?Mn binary oxide adsorbent can be regenerated by treating with3mol/L NaOH,and the W adsorption efficiency was retained after five adsorption?desorption?regeneration cycles.All these indicate that the Fe?Mn binary oxides have the potential for the separation of W from molybdate solution.

Experimental study on the inhibition of biological reduction of Fe(III)EDTA in NO_x absorption solution

Scrubbing of NOx from the gas phase with Fe(II)EDTA has been shown to be highly effective. A new biological method can be used to convert NO to N2 and regenerate the chelating agent Fe(II)EDTA for continuous NO absorption. The core of this biological regeneration is how to effectively simultaneous reduce Fe(III)EDTA and Fe(II)EDTA-NO, two mainly products in the ferrous chelate absorption solution. The biological reduction rate of Fe(III)EDTA plays a main role for the NOx removal efficiency. In this paper, a bacterial strain identified as Klebsiella Trevisan sp. was used to demonstrate an inhibition of Fe(III)EDTA reduction in the presence of Fe(II)EDTA-NO. The competitive inhibition experiments indicted that Fe(II)EDTA-NO inhibited not only the growth rate of the iron-reduction bacterial strain but also the Fe(III)EDTA reduction rate. Cell growth rate and Fe(III)EDTA reduction rate decreased with increasing Fe(II)EDTA-NO concentration in the solution.

基于柔性配体5-[N-乙酸根(4-吡啶基)]四唑(a4-pytz)与Fe(II)和Sm(III)两个配合物的合成与表征

5-[N-乙酸根(4-吡啶基)]四唑钾盐(简写为Ka4-pytz)与(NH4)2Fe(SO4)2和SmCl3·6H2O在水-甲醇体系中反应,得到两个新的配合物,[Fe(a4-pytz)2·2H2O]·2H2O (1)和[Sm4(a4-pytz)8(H2O)18]Cl3·10H2O (2)。通过元素分析,红外光谱分析及X-射线单晶衍射对两个配合物进行结构表征。单晶衍射结果显示了配合物1和2都具有一维链状结构。但不同的是,配合物1的一维链是通过a4-pytz作为双齿配体,经四唑环上的氮原子和羧基的一个氧原子与Fe(II)相连而成的;而配合物2的结构形成源于羧基的桥联作用,氮原子未配位。通过氢键作用,配合物1和2形成了三维结构。室温下研究了配合物1和2的荧光性质。

Photooxidation of Methacrolein in Fe(III)-Oxalate Aqueous System and Its Atmospheric Implication

Iron and oxalic acids are widely distributed in the atmosphere and easily form ferric oxalate complex(Fe(III)-Ox).The tropospheric aqueous-phase could provide a medium to enable the photo-Fenton reaction with Fe(III)-Ox under solar irradiation.Although the photolysis mechanisms of Fe(III)-Ox have been investigated extensively,information about the oxidation of volatile organic compounds(VOC),specifically the potential for Secondary Organic Aerosol(SOA)formation in the Fe(III)-Ox system,is lacking.In this study,a ubiquitous VOC methacrolein(MACR)is chosen as a model VOC,and the oxidation of MACR with Fe(III)-Ox is investigated under typical atmospheric water conditions.The effects of oxalate concentration,Fe(III)concentration,MACR concentration,and pH on the oxidation of MACR are studied in detail.Results show that the oxidation rate of MACR greatly accelerates in the presence of oxalate when compared with only Fe(III).The oxidation rate of MACR also accelerates with increasing concentration of oxalate.The effect of Fe(III)is found to be more complicated.The oxidation rate of MACR first increases and then decreases with increasing Fe(III)concentration.The oxidation rate of MACR increases monotonically with decreasing pH in the common atmospheric water pH range or with decreasing MACR concentration.The production of ferrous and hydrogen peroxide,pH,and aqueous absorbance are monitored throughout the reaction process.The quenching experiments verify that·OH and O_(2)^(+)are both responsible for the oxidation of MACR.MACR is found to rapidly oxidize into small organic acids with higher boiling points and oligomers with higher molecular weight,which contributes to the yield of SOA.These results suggest that Fe(III)-Ox plays an important role in atmospheric oxidation.

石煤含氟酸浸液中V(Ⅴ)-Fe(Ⅲ)-F-H_(2)O系钒铁分离热力学研究

针对石煤含氟酸浸液中钒铁分离问题,计算并绘制298.15 K下V(Ⅴ)-Fe(Ⅲ)-F-H_(2)O系热力学平衡图,分析含钒离子、含铁离子随总钒浓度、总铁浓度、总氟浓度的变化规律。研究结果表明,随着pH由0升高至3.00,由于氟离子与VO_(2)^(+)、Fe^(3+)的配位作用,含钒物种由阳离子转变为阴离子,含铁物种由阳离子转变为中性分子,此时可实现钒铁有效分离。定义pH_(50%)为含钒阴离子摩尔分数50%时的pH,溶液中总钒浓度升高、总铁浓度升高,均导致pH50%升高,总氟浓度升高,pH_(50%)则降低。采用N235阴离子萃取剂分离含氟溶液中的钒铁,当溶液中总钒浓度为0.05 mol/L、总铁浓度为0.05 mol/L、总氟浓度为0.50 mol/L时,溶液萃取pH升高,钒铁分离系数βV/Fe增加,当pH为1.97时,钒铁分离系数β_(V/Fe)可达122.86,钒铁达到有效分离,与热力学分析结果一致。