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1.
为了探究热活化过硫酸盐（PS）技术对水中氧氟沙星（OFX）的氧化降解作用,考察了反应温度、体系的初始pH、PS的初始浓度、OFX的初始浓度对OFX降解效果的影响;并在单因素实验的基础上,选取反应时间、体系的初始pH、PS的初始浓度和OFX的初始浓度4个因素进行了响应面优化实验。结果表明：最佳降解条件为,反应温度60℃、PS初始浓度4.0 mmol/L、pH=4.7、OFX初始浓度0.03 mmol/L、反应时间60 min,此时OFX的降解率为81.29%;4个因素对热活化PS降解OFX均有影响,其影响显著性从大到小为反应时间、OFX的初始浓度、PS的初始浓度、初始pH。利用响应曲面法模拟出反应体系的最佳条件,经实验验证,OFX降解率为93.78%,与预测最佳结果95.00%基本相符,表明模型可靠有效。 相似文献
2.
近期见有含二价铁矿物可活化分子氧产生羟自由基而氧化污染物的报道。本文选用土壤/沉积物中的常见组分蒙脱石(含铁约2%),研究了还原态蒙脱石在不同条件下活化分子氧降解苯酚的效果。结果表明,20g/L还原态蒙脱石(还原程度为30%)在pH=6和有氧条件下,可通过产生羟自由基使11μM苯酚的降解率在6h内持续增加至59.1%。苯酚降解率对应的最佳pH为5,当pH>6时降解率则随着p H的升高而急剧降低;苯酚降解效果还随还原态蒙脱石剂量(0~40g/L)增加而提高;苯酚初始浓度为11μM降解率最高,增加或者降低初始浓度均使降解率降低。还原态蒙脱石铁含量低,活化分子氧时其八面体边缘配位和结构内部二价铁共同起作用,而受八面体层Al、Mg等惰性组分阻碍,其结构二价铁难以向边缘位置传递电子,这与前期报道的还原态绿脱石(含铁约20%)不同。 相似文献
3.
基于硫酸根自由基的高级氧化技术能有效降解水中磺胺类药物残留。由于在自然环境中共存重金属会对环境修复效果产生一定影响,文中重点研究了不同pH环境条件下不同重金属离子对针铁矿活化过硫酸盐(PS)去除水中磺胺吡啶(SPY)的影响。不同类型重金属离子(Cu^2+、Pb^2+、Cd^2+,0.2mmol/L)在反应体系(初始条件:针铁矿,1.0g/L;PS,4mmol/L;SPY,10mg/L;pH=8.2)中对SPY的降解对比研究发现:在无重金属共存的条件下,针铁矿/PS体系降解SPY的去除率为25.2%;Pb^2+和Cd^2+对针铁矿/PS体系的影响较弱,去除率分别为30.8%和34.8%;Cu^2+的促进作用很大,可以使SPY被完全降解(100%)。机理分析认为,在针铁矿/PS体系中Pb^2+和Cd^2+主要通过影响吸附作用导致磺胺吡啶被去除,而Cu^2+主要通过自身活化PS的作用。不同pH条件(3.0,8.0,12.0)实验证实弱碱性条件下,Cu^2+/针铁矿/PS能够发挥较高的活性从而降解SPY。本文结果为采用针铁矿活化过硫酸盐技术修复类似复合污染地下水环境提供了实验依据。 相似文献
4.
本文采用超声强化零价铁活化过硫酸盐氧化降解地下水中的二恶烷污染物。主要探讨了零价铁添加量、超声强化、不同过硫酸盐用量及地下水中不同碳酸根浓度等对二恶烷降解效果的影响,并对零价铁进行了表征分析。结果表明：超声能够促进硫酸根自由基和Fe2+的产生,提高二恶烷的降解率;零价铁添加量和过硫酸盐浓度的增加均能促进二恶烷的降解,但零价铁相对过硫酸盐过多时将降低最终降解率;地下水中的碳酸根会消耗硫酸根自由基,因此碳酸根浓度越高,二恶烷降解率越低。超声强化零价铁活化过硫酸盐氧化法能够有效降解二恶烷,并具有应用于处理地下水中二恶烷的潜力。 相似文献
5.
三氯乙烯（TCE）是一种地下水中常见的有机污染物，传统的地下水循环井修复技术虽然有效但耗时长，且需配套地面处理。文章研发了一种电化学循环井耦合修复体系，以期通过顺序化学氧化 -还原作用高效快速降解地下水中TCE。以地下水循环井为基础，通过抽水井中的地下水电解，原位提供O2和H2，投加Fe（Ⅱ） -EDTA络合物活化O2产生羟基自由基氧化降解TCE，进而利用钯催化剂催化剩余的H2还原降解TCE。在二维砂槽模拟含水层中评价了该体系的运行效果，含水层中初始TCE浓度为7.50 mg/L，经过13天的连续通电处理后，TCE浓度降低到1.65 mg/L，降解率达到78%。处理后Cl-浓度相应增加118.20 μmol/L，接近于TCE降解量（44.50 μmol/L）的3倍，证明TCE近乎完全脱氯。运行过程中，TCE平均降解速率由0~5 d的0.90 mg/(L·d) 降低到9~13 d的0.10 mg/(L·d)，氧化降解主要发生在前期阶段，钯催化还原效率较为稳定，后期两种过程降解效率都逐渐下降，主要原因是溶解态Fe（Ⅱ）浓度减少以及钯催化剂活性降低。该耦合修复体系是基于地下水循环井技术的改进，其氧化 -还原作用机理有望实现地下水中多种不同有机污染物的降解。 相似文献
6.
硫酸根自由基的高级氧化技术以高效率、污染少等优点被广泛用于环境污染治理。本文以实际石油污染土壤为对象,运用该体系对土壤进行修复研究,分别从Na_2S_2O_8/Fe~(2+)摩尔比、体系pH值、Na_2S_2O_8/Fe~(2+)投加量等方面开展了实验研究。实验表明:当Na_2S_2O_8/Fe2+摩尔比为2∶3时,石油污染物的降解效果最好,体系的pH值对降解效果影响不大,1 g土壤中浓度为0.1 mol/L的过硫酸钠和硫酸亚铁溶液的最佳加入量为2 m L、3 m L时,对土壤的降解效果最为明显,故每吨污染土壤的添加量大约为2×10~6m L、3×10~6m L。 相似文献
7.
为了进一步研究氮掺杂碳材料活化过硫酸盐降解4-氯苯酚的方法，首先以廉价易得的废弃工业糖浆作为碳源，以氨水作为氮源，利用溶胶-凝胶法合成了3种氮掺杂碳材料（NC-700，NC-800和NC-900），并利用扫描电子显微镜（SEM）、X射线衍射（XRD）、拉曼光谱（Raman）、X射线光电子能谱（XPS）等技术对氮掺杂碳材料进行表征分析；然后考察了NC-800投加量、过硫酸盐（PDS）投加量和初始pH等因素对4-氯苯酚去除率的影响，并进行了电子自旋共振（ESR）和自由基淬灭实验。结果表明：3种材料均可有效活化PDS降解4-氯苯酚，其中NC-800活化PDS去除4-氯苯酚效率最高；当NC-800投加量为100 mg/L、PDS投加量为5 mmol/L时，反应30 min后，50 mg/L的4-氯苯酚的总去除率达99.10%；初始pH对4-氯苯酚去除率无明显影响；NC-800活化过硫酸盐降解4-氯苯酚遵循非自由基途径，单线态氧为降解4-氯苯酚的活性物质。循环使用实验证明NC-800具有一定的稳定性，4次循环使用后，4-氯苯酚去除率仍可达到73.80%。 相似文献
8.
研究了山西代县天然金红石在紫外光和日光照射条件下对苯酚的光催化降解性能,考察了光照时间、pH值、苯酚初始浓度以及H2O2添加量对降解过程的影响。在紫外光照射下,酸性条件(pH=3.5)利于光催化降解,中性和碱性条件下降解效率较低;当初始浓度为60mg/L时,降解速率可达1.922mg/(L.h);H2O2作为电子捕获剂可提高苯酚降解速率,最佳投加量为2mL/L。在日光条件下,天然金红石对苯酚表现出良好的降解性能,照射7h后,降解率达87.68%,仅略低于P25型TiO2(99.72%),可在14h内完全降解。根据电子探针和X射线衍射分析结果,认为天然金红石晶格中的V、Fe等杂质可能是提高其可见光响应效果和光催化活性的主要原因。 相似文献
9.
研究了La0.5 Sr0.5 Co0.8 Mn0.2 O3-δ钙钛矿活化过氧单硫酸盐对四溴双酚A(TBBPA)的降解作用,重点探讨不同的煅烧温度制备镧锶钴锰钙钛矿(LSCM82)的催化性能对过一硫酸盐降解TBBPA的影响,以及溶液的不同初始pH条件对优选材料体系降解效率的影响。结果发现,变价离子的氧化还原对Co3+/Co2+和(Mn4++Mn3+)/Mn2+是催化剂活性的主要贡献者。煅烧温度为950 ℃且具有适量间隙氧及比表面积的LSCM82-950催化反应速率较高。在中性pH环境条件下应用LSCM82-950活化过一硫酸盐降解水中TBBPA污染物,既可以使催化剂钴浸出很少,又能达到最大程度的TBBPA降解效果。 相似文献
10.
掺铁二氧化钛薄膜的自组装制备、表征与光催化性能研究 总被引：3，自引：0，他引：3
采用自组装方法于低温液相反应体系中成功制备出大尺寸二维纳米二氧化钛薄膜和掺铁二氧化钛薄膜。样品通过荧光发射光谱、拉曼光谱、高分辨透射电镜等方法进行表征,并研究了紫外光和可见光下Fe3+/TiO2纳米薄膜对甲基橙溶液(MO)的光催化降解过程,探讨了Fe3+对TiO2的光催化活性的影响。结果表明,此方法不需要高温煅烧即可得到高催化活性的金红石和锐钛矿混合型二氧化钛薄膜,以金红石为主。Fe3+掺杂明显提高了TiO2对甲基橙溶液的光催化降解效率:掺杂Fe3+浓度为0.5 mmol/L时光催化效果最优,且更利于较低浓度甲基橙溶液的降解,在紫外光和可见光下对初始浓度5 mg/L甲基橙溶液的降解率分别达到98.62%和89.24%。 相似文献
11.
J. Deng Y. Shao N. Gao Y. Deng C. Tan S. Zhou 《International Journal of Environmental Science and Technology》2014,11(4):881-890
Zero-valent iron (Fe0), as an alternative iron source, was evaluated to activate persulfate (PS) to degrade acetaminophen (APAP), a representative pharmaceutically active compound in water. Effects of key factors in the so-called Fe0/PS process, including Fe0 dosage, initial pH, temperatures and chelating agents, were studied. Under all the conditions tested, the APAP degradation followed a pseudo-first-order kinetics pattern. The degradation efficiency of APAP was highest when the Fe0 to PS molar ratio increased to 1:1, and the degradation rate constant and removal were 23.19 × 10?3 min?1 and 93.19 %, respectively. Comparing with Fe2+, Fe0 served as an alternative iron source that can gradually release Fe2+ into water, thereby consistently activating PS to produce sulfate radicals. The Fe0/PS system was effective in a broader pH range from 3 to 8.5. Heat could facilitate production of sulfate radicals and enhance the APAP degradation in the Fe0/PS system. High reaction temperature also improved the Fe2+/PS oxidation of APAP. Finally, sodium citrate (a chelating agent) at an appropriate concentration could improve the APAP degradation rate in the Fe2+/PS and Fe0/PS system. The optimal molar ratio of Fe0 to citrate depended on solution pH. Our results demonstrated that Fe0 was an alternative iron source to activate PS to degrade APAP in water. 相似文献
12.
为探讨不同碳氮源对培养基中铀酰离子的络合形态及荧光假单胞菌对铀吸附和还原作用的影响,本文以查氏培养基为基础,将蔗糖替换为葡萄糖或将硝酸钠替代为氯化铵,采用Visual MINTEQ分析研究铀酰离子络合形态。研究结果表明,碳氮源的种类对微生物生长无影响。U(Ⅵ)浓度为10 mg/L时,3种培养基中铀酰离子的主要络合形态均为UO2PO-4。U(Ⅵ)浓度为50~200 mg/L,查氏和葡萄糖碳源培养基中铀酰离子主要络合形态均为UO2(SO4)2-2。氯化铵氮源培养基中,U(Ⅵ)浓度为50 mg/L时铀酰离子的主要络合形态为UO2HPO4(aq),浓度为100~200 mg/L时主要是UO2Cl2(aq)。荧光假单胞菌对U(Ⅵ)耐受浓度高达100 mg/L,当U(Ⅵ)浓度达到200 mg/L时,菌体失活。荧光假单胞菌为活体时,对U(Ⅵ)的吸附率为84.02%~92.59%,还原率为3.32%~10.94%,不同碳氮源对铀吸附和还原的影响较小。荧光假单胞菌为死体时,对铀的吸附率为24.33%~39.05%;非葡萄糖碳源培养基中,对铀的还原率为37.50%~44.58%,含还原性葡萄糖的培养基条件下U(Ⅵ)的还原率为53.12%。还原性葡萄糖与荧光假单胞菌对铀的还原为协同作用。荧光假单胞菌为活体时,培养基成分被微生物充分利用,两者协同作用不明显。 相似文献
13.
Natural specimens of green gemological euclase (chemical formula BeAlSiO4(OH)) from Brazil were investigated by electron paramagnetic resonance (EPR) and optical absorption. In addition to iron-related
EPR spectra, analyzed recently in blue and colorless euclase, chromium and vanadium-related EPR spectra were also detected
in green euclase. Their role as color causing centers is discussed. The results indicate that Cr3+ ions substitute for Al3+ ions in the euclase structure. The EPR rotation patterns of Cr3+ with electron spin S = 3/2 were analyzed with monoclinic spin Hamiltonian leading to the parameters of g
xx
, g
yy
and g
zz
equal to 2.018, 2.001 and 1.956 and electronic fine structure parameters of D = −8.27 GHz and E = 1.11 GHz, respectively, with high asymmetry ratio E/D = 0.13. For the vanadium-related EPR spectra the situation is different. It is concluded that vanadium is incorporated as
the vanadyl radical VO2+ with electron spin S = 1/2 with nearly axial spin Hamiltonian parameters gzz = 1.9447, g
xx
= 1.9740 g
yy
= 1.9669 and axial hyperfine interactions due to the nuclear spin I = 7/2 of the 51V isotope leading to A
zz
= 502 MHz, A
xx
= 150 MHz and A
yy
= 163 MHz. The green color of euclase is caused by two strong broad absorption bands centered at 17,185 and 24,345 cm−1 which are attributed to the 4A2g → 4T2g, 4T1g transitions of Cr3+, respectively. Vanadyl radicals may introduce some absorption bands centered in the near infrared with tail extending into
the visible spectral range. 相似文献
14.
Experimental evidence is reported for Fe2+ disproportionation in Al-free perovskite (Pv), when submitted to large temperature gradients (i.e., under off-equilibrium
conditions) in a laser heated diamond anvil cell (LHDAC). To enable this effect, the experimental procedure was designed to
produce large radial and axial temperature gradients. In the Pv and ferropericlase (Fp) assemblage synthesized after dissociation
of natural olivine, the three chemical states of iron (i.e., Fe0, Fe2+ and Fe3+) could be evidenced by electron probe microanalysis (EPMA), through variations of oxygen contents attached to the Fe cations.
Despite inherent difficulties for determination of O-contents and Fe3+/ΣFe ratios using EPMA, we recorded significant changes in iron oxidation state across the laser-heated strip. These changes
are correlated with variations in composition for the major elements (Fe, Mg, and Si), which evidences that the Pv/Fp assemblage
experienced large segregation under the strong temperature gradients. Grains of metallic iron were detected in parts of the
laser-heated strip coexisting with a Pv phase with Fe/(Mg + Fe) = 6 at% and most of its iron as Fe3+. This Fe2+-disproportionation reaction involves insertion of Fe3+-defects in the Pv lattice. This Fe3+-bearing Pv phase is presumably unstable and decomposes into a mineral assemblage including magnesioferrite, which is detected
at the border of the laser-heated strip. 相似文献
15.
羟自由基(·OH)是自然环境中氧化活性最强的物种,对物质转化具有重要影响.前期研究发现地下水接触O2可产生·OH,其中Fe2+氧化起主导作用,但地下水化学组成对Fe2+氧化产生·OH的影响尚不清楚.通过室内模拟实验,探究了地下水中常见组分(Ca2+、Mg2+、腐殖酸(HA)和磷酸根)对Fe2+氧化产生·OH的影响.结果表明,pH 6.5时0.357 mM Fe2+在5 h内氧化完全,产生约1.8 μM的·OH;Ca2+(1~6 mM)、Mg2+(1~4 mM)对Fe2+氧化和·OH产生无明显影响;HA(10~30 mg/L)促进Fe2+氧化和·OH产生,促进效果随pH降低而增强;磷酸根(0.01~0.03 mM)抑制Fe2+氧化,对·OH产生的影响为先抑制后促进. 相似文献
16.
为研究双金属催化剂去除有机污染物的效果,采用自制Fe/Ag催化剂对模拟苯酚废水进行了臭氧催化氧化处理。通过扫描电子显微镜(SEM)、比表面积分析仪(BET)和X射线衍射(XRD)对催化剂进行表征,并考察了催化剂类型、催化剂投加量和溶液初始pH值对降解效果的影响规律。结果表明:与Fe相比,Fe/Ag比表面积减少了22.8%,在Fe/Ag/O3与含苯酚废水的反应体系中,反应遵循臭氧直接作用和活性自由基(·OH、·O2、H2O2)共同作用的机理;Fe/Ag在反应过程中体现出良好的协同作用;300 mg/L的苯酚模拟废水在pH=6.3、Fe/Ag投加量为1.00 g的最优反应条件下经60 min反应,苯酚与化学需氧量(COD)去除率比单独臭氧氧化分别提高了18.4%和29.4%。 相似文献
17.
Thomas Pichler 《Environmental Geology》2005,47(2):215-224
The application of sulfur isotope (34S) values of sulfate in groundwater provided the information necessary to evaluate the source, transport and fate of battery acid and associated contaminants at the Gulf Coast Recycling (GCR) facility. The chemical and isotopic composition of groundwater beneath the (GCR) property, a battery recycling facility in east Tampa, Florida, varies more than expected for an area of comparable size. Sulfate (SO42–) values, for example, range from 1.2 to 11,500 mg/L and oxygen and hydrogen isotopes do not attenuate towards the weighted annual mean. Those samples that are high in sulfate generally have a low pH, which immediately indicates battery acid (H2SO4) contamination as a potential source for the sulfate. The low pH and high reactivity of the sulfuric acid groundwater cause the formation of hydrogeological microenvironments due to preferential dissolution of carbonate minerals, which in turn causes enhanced recharge and groundwater flow in certain areas; thus, the extreme scatter in the data set. Because of the difficult hydrogeology it is not straightforward to delineate the point-sources of contamination and up to five potential scenarios have to be evaluated: (1) seawater intrusion, (2) upwelling of high-sulfate groundwater, (3) local dissolution of gypsum, (4) an up-gradient contaminant source to the northeast of the GCR property and (5) battery acid contamination. 相似文献