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11.
铁铜双金属有机骨架MIL-101(Fe,Cu)活化双氧水降解染料性能 总被引:1,自引:0,他引:1
针对非均相芬顿传质效率低和Fe(Ⅲ)Fe(Ⅱ)转化慢导致活性低等问题,采用溶剂热法制备铁铜双金属有机骨架材料[MIL-101(Fe,Cu)],并研究了材料界面性质、催化降解染料(亚甲基蓝)性能以及活化催化机制.结果表明,MIL-101(Fe,Cu)晶体结构完整且呈三维八面体形状;比表面积和平均孔径分别为667.2 m2 ·g-1和1.9 nm,可充分暴露反应活性位点.MIL-101(Fe,Cu)在广谱pH范围可活化H2 O2高效降解亚甲基蓝.当pH=5、反应20 min,MIL-101(Fe,Cu)/H2 O2对20 mg ·L-1亚甲基蓝的去除率为100%,较MIL-101(Fe)/H2O2和单独H2 O2分别提高43.1%和88.9%.自由基猝灭实验与反应前后铁和铜价态变化结果表明,羟基自由基(·OH)是MIL-101(Fe,Cu)/H2 O2催化降解亚甲基蓝的主要活性物种;Cu(Ⅱ)掺杂引入新的活性位点,且Cu(Ⅱ)/Cu(Ⅰ)循环和Fe(Ⅲ)/Fe(Ⅱ)循环可协同产生·OH,进而提高催化效率.MIL-101(Fe,Cu)作为新型非均相类芬顿催化剂,无需复杂pH调节即可获得良好催化效果,在工业废水处理上具有较好地应用前景. 相似文献
12.
树脂负载Fe3+/Cu2+多相类芬顿降解染料橙黄 总被引:3,自引:1,他引:2
制备了新型多相类Fenton催化剂(Fe3+cu2+)/R(Fe3+和cu2+同时负载于离子交换树脂),以橙黄Ⅳ为研究对象,探讨了初始过氧化氢浓度、橙黄Ⅳ浓度、催化剂量、初始pH值及温度等因素对催化反应速率的影响,并对该催化剂重复使用性能进行测试.研究结果表明,该催化剂(Fe3++Cu2+)/R与Fe3+/R相比表现出更好的催化过氧化氢分解的活性,使橙黄Ⅳ的降解率提高10%;催化过氧化氢氧化橙黄Ⅳ的反应遵循假一级反应动力学,反应活化能为10.71 kJ·mol-1;催化剂表现出良好的重复使用性能,Fe3+和cu2+在树脂表面负载比较牢固,具有较好的稳定性和耐用性.同时,电子顺磁共振(EPR)测试结果表明,cu2+的掺杂能有效地促进OH·的产生;X射线光电子能谱(XPS)测试结果表明,反应过程中存在高价态铁物种.因此,在该体系反应过程中产生的活性物种是OH·和高价态铁同时共存. 相似文献
13.
采用水热法合成了Fe-MCM-41中孔分子筛,紫外、红外及XRD表征显示铁离子已进入中孔分子筛骨架。以H2O2为氧化剂形成类Fenton试剂,实验结果表明,在催化剂加入量为1 g/L、H2O2体积分数为6%、pH为4、反应时间为10h、反应温度为35℃的条件下,处理质量浓度为50 mg/L的2,4-D废水的降解率达94.95%。宏观动力学研究显示,该反应近似为一级反应,反应速率常数、表观活化能分别为0.21667 min-1和26.65 kJ/mol。 相似文献
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15.
楼静 《中国环境管理干部学院学报》2004,14(3):38-39
利用由O2和Fenton试剂组成的类Fenton系统处理对氨基苯磺酸废水,取得了很好的降解效果.当FeSO4(10g/L)投加量为1.2mL、H2O2(3%)投加量为3mL时,COD去除率可达到70%. 相似文献
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Siedlecka EM Stepnowski P 《Environmental science and pollution research international》2009,16(4):453-458
Background, aim, and scope Ionic liquids are regarded as essentially “green” chemicals because of their insignificant vapor pressure and, hence, are
a good alternative to the emissions of toxic conventional volatile solvents. Not only because of their attractive industrial
applications, but also due to their very high stability, ionic liquids could soon become persistent contaminants of technological
wastewaters and, moreover, break through into natural waters following classical treatment systems. The removal of harmful
organic pollutants has forced the development of new methodologies known as advanced oxidation processes (AOPs). Among them,
the Fenton and Fenton-like reactions are usually modified by the use of a higher hydrogen peroxide concentration and through
different catalysts. The aim of this study was to assess the effect of hydrogen peroxide concentration on degradation rates
in a Fenton-like system of alkylimidazolium ionic liquids with alkyl chains of varying length and 3-methyl-N-butylpyridinium chloride.
Materials and methods The ionic liquids were oxidized in dilute aqueous solution in the presence of two different concentrations of hydrogen peroxide.
All reactions were performed in the dark to prevent photoreduction of Fe(III). The concentrations of ionic liquids during
the process were monitored with high-performance liquid chromatography. Preliminary degradation pathways were studied with
the aid of 1H NMR.
Results Degradation of ionic liquids in this system was quite effective. Increasing the H2O2 concentration from 100 to 400 mM improved ionic liquid degradation from 57–84% to 87–100% after 60 min reaction time. Resistance
to degradation was weaker, the shorter the alkyl chain.
Discussion The compound omimCl was more resistant to oxidation then other compounds, which suggests that the oxidation rates of imidazolium
ionic liquids by OH· are structure-dependent and are correlated with the n-alkyl chain length substituted at the N-1-position. The level of degradation was dependent on the type of head group. Replacing
the imidazolium head group with pyridinium increased resistance to degradation. Nonetheless, lengthening the alkyl chain from
four to eight carbons lowered the rate of ionic liquid degradation to a greater extent than changing the head group from imidazolium
to pyridinium. 1H-NMR spectra show, in the first stage of degradation, that it is likely that radical attack is nonspecific,
with any one of the carbon atoms in the ring and the n-alkyl chain being susceptible to attack.
Conclusions The proposed method has proven to be an efficient and reliable method for the degradation of imidazolium ionic liquids by
a Fenton-like reagent deteriorated with lengthening n-alkyl substituents and by replacing the imidazolium head group with pyridinium. The enhanced resistance of 1-butyl-3-methylpyridinium
chloride when the resistance of imidazolium ionic liquids decreases with increasing H2O2 concentration is probably indicative of a change in the degradation mechanism in a vigorous Fenton-like system. H-NMR spectra
showed, in the first stage of degradation, that radical attack is nonspecific, with any one of the carbon atoms in the ring
and the n-alkyl chain being susceptible to attack.
Recommendations and perspectives Since ionic liquids are now one of the most promising alternative chemicals of the future, the degradation and waste management
studies should be integrated into a general development research of these chemicals. In the case of imidazolium and pyridinium
ionic liquids that are known to be resistant to bio- or thermal degradation, studies in the field of AOPs should assist the
future structural design as well as tailor the technological process of these chemicals 相似文献
18.
研究了微波辐射下Cr(VI)-H2O2催化降解甲基橙溶液的行为,探索了微波功率、微波辐射时间、pH值、H2O2浓度、Cr(VI)等对甲基橙溶液脱色率和COD去除率的影响。研究结果表明,Cr(VI)-H2O2能形成类Fenton体系;微波辐射可提高H2O2产生羟基自由基(·OH)的效率。1000 mg/L的甲基橙溶液,在Cr(VI)浓度为10.0 mmol/L、pH值为2.5、H2O2浓度为20.0 mmol/L、微波功率为700W下加热2 min,甲基橙溶液的脱色率为99.2%,COD去除率为82.8%。 相似文献
19.
Shicheng Wei Cuiping Zeng Yaobin Lu Guangli Liu Haiping Luo Renduo Zhang 《Frontiers of Environmental Science & Engineering》2019,13(5):66
20.
Hang Zhang Shuo Chen Haiguang Zhang Xinfei Fan Cong Gao Hongtao Yu Xie Quan 《Frontiers of Environmental Science & Engineering》2019,13(2):18