共查询到18条相似文献,搜索用时 218 毫秒
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利用共价三嗪有机框架材料(CTF-1)对4-氯酚(4-CP)、2,4-二氯酚(2,4-DCP)、2,4,6-三氯酚(2,4,6-TCP)和五氯酚(PCP)等4种不同氯原子取代数目的氯酚类污染物进行光催化降解研究,探讨了底物结构对氯酚脱氯降解效率的影响及机制.结果表明,氯酚脱氯降解过程明显受苯环氯原子取代数目的影响,氯原子数目越多,脱氯降解效率越高,氯原子数目与表观速率常数呈显著正相关,氯酚降解及脱氯速率均为:PCP>2,4,6-TCP>2,4-DCP>4-CP.对CTF-1光催化降解氯酚机制研究表明,活性物种在反应中不起作用,体系反应机制为针对氯酚上取代氯位点进行水解脱氯过程.本研究结果为深入揭示氯酚脱氯降解机制提供了理论依据,也为光催化技术处理卤代酚类废水提供了技术参考. 相似文献
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多氯联苯是一种典型的持久性有机污染物,其在环境中的转化归趋备受关注.在厌氧条件下,多氯联苯可以通过微生物脱氯进行降解,该降解方式虽然广泛存在于自然界中,但是受生物地球化学因素的影响较大,调控较为复杂.本文对多氯联苯的厌氧微生物脱氯降解进行综述,讨论了脱氯路径和自然界中8种主要脱氯历程;脱氯微生物及相关的微生物还原脱卤酶;影响脱氯速率、程度和历程的主要物理和地球化学因素(温度、pH和氧化还原水平、碳源、电子受体、电子供体及抑制物).最后分析了多氯联苯厌氧脱氯研究中存在的问题并对其前景进行展望. 相似文献
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零价铁对土壤中4-氯苯酚还原脱氯研究 总被引:12,自引:2,他引:12
氯苯酚是常见的环境污染物,它们在土壤中的加速分解可以减少对人类健康的危害。以恒温培养为方法,GC-MS为检测手段,研究了在常温常压下土壤中4-氯苯酚(4-CP)在零价铁作用下的还原脱氯反应。结果表明:4-CP可以被来自零价铁的电子还原,零价铁能够有效促进土壤中的4-CP脱除苯环上的氯原子,从而达到降低毒性、增加可生化性目的。反应条件如初始pH、时间、零价铁用量等均对4-CP还原脱氯效率有重要影响,特别是当初始pH值控制在偏酸时更有利于反应的进行。在零价铁加入量500mg、初始pH=4、反应时间7d的条件下,零价铁对土壤中4-CP还原脱氯效率最高可以达到65%。利用实验数据,对零价铁作用下4-CP还原脱氯的反应机理也进行了初步探讨。 相似文献
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厌氧颗粒污泥对五氯苯酚脱氯过程中的影响因素 总被引:1,自引:1,他引:1
在间歇培养血清瓶中,研究了厌氧颗粒污泥对五氯酚脱氯过程中的影响因素.结果表明,葡萄糖、酵母膏和蛋白胨显著提高了PCP的脱氯速率.添加甲酸、乙酸、乙醇对PCP脱氯速率有一定提高,丙酸和丁酸对脱氯速率没有影响.20%氢气的加入对PCP脱氯速率的影响显著.废水中硝酸盐和硫酸盐等电子受体的存在降低了PCP的脱氯速率.微生物抑制剂氯仿、青霉素降低了PCP脱氯速率,表明厌氧微生物尤其是甲烷菌对还原脱氯有重要影响.PCP最佳还原脱氯温度为38℃,最佳pH为7,低的氧化还原电位(<-200mV)有利于脱氯的进行.图5参13 相似文献
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自然环境中,大多数氯代有机污染物厌氧还原脱氯反应是与土壤环境中一些生源要素的生物化学还原过程相伴生。有机污染物的种类、生物有效性以及毒性能够显著影响这些生源要素的转化,反过来,土壤中活跃的氧化还原反应也可以显著影响有机污染物的动力学转化过程。本文从氧化还原顺序上综述了反硝化过程、铁还原过程、硫酸盐还原过程和产甲烷过程对氯代有机污染物厌氧还原脱氯过程的影响与作用机制,旨在为氯代有机污染物在厌氧环境中还原脱氯的过程与机理的进一步研究、以及还原脱氯与微生物介导的生源要素氧化还原过程的耦合作用机制的揭示提供参考。 相似文献
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采用共浸渍法制备了一系列Al2O3负载金属Pd、Cu催化剂.通过元素分析(ICP)、氮气吸脱附(BET)、X射线粉末衍射(XRD)、透射电镜(TEM)等技术对催化剂进行了表征,并以1,2-二氯乙烷气相加氢脱氯为探针反应,考察了Pd-Cu/Al2O3催化剂的钯铜比、反应温度、反应时间等因素对催化活性以及反应产物乙烯选择性的影响.结果发现,提高Cu负载量可在催化剂中形成Pd-Cu合金,并促进催化剂对乙烯的选择性.此外,当温度为250℃,Pd、Cu负载量分别为0.78%和1.9%时的Pd-Cu/Al2O3催化剂对1,2-二氯乙烷的催化加氢脱氯效果最佳,最终产物乙烯的选择性可达到80%以上. 相似文献
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In this study, polychlorinated biphenyls (PCBs) were decomposed by low‐temperature heat treatment with metallic catalyst, and with metallic catalyst and a hydrogen source. Of the catalysts used, iron (Fe) was the most active catalyst for the decomposition of PCBs, and the decomposition was due to dechlorination. The addition of hydrogen sources accelerated the decomposition of PCBs in the presence of catalyst. Surface analysis of the catalyst using X‐ray photoelectron spectroscopy (XPS) suggested that the emitted chlorine was presumed to form metal chloride. The reactions of each homolog can be expressed by a successive first‐order reaction model. This means that a substituted chlorine is successively detached during this reaction. The overall decomposition rate in this reaction system was controlled by that of the lower chlorinated homologs. The decomposition rates with Fe and NaBH4 for the lower chlorinated homologs were about 10 times as fast as the rates with only Fe. 相似文献
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Xin Xing Na Li Dandan Liu Jie Cheng Zhengping Hao 《Frontiers of Environmental Science & Engineering》2022,16(10):125
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The present work, in which cellulose isolated from formic acid fractionation (FAC) is decorated with polyetherimide (PEI) to attain highly efficient cellulose-derived PdAgbimetallic catalyst (PdAg-PEI-FAC), has been investigated, and the catalyst properties are characterized by XRD, XPS, BET, ICP-AES and HAADF-STEM. The as-obtained Pd3.75Ag3.75-PEI-FAC exhibits excellent catalytic performance for H2 evo-lution from a sodium formate-free formic acid (FA) aqueous medium at ambient temperature and the turnover frequency (TOF) reaches a high value of 2875 h-1, which is superior to most of the previously reported Pd-based heterogeneous catalysts supported on a carbon matrix in the literature. The remarkable catalytic activities of PdAg-PEI-FAC result from high dispersion Pd and synergistic effects between the PdAg bimetallic system. Furthermore, the amide (-NH) group in PEI coated on cellulose acting as a proton scavenger efficiently improves the catalytic property of catalyst. In addition, the critical factors affecting H2 release, such as FA concentration, reaction temperature, PdAg compositions and support matrix type, are also evaluated. Based on the experimental results, the probable three-step mechanism of H2 evolution from FA over Pd3.75Ag3.75-PEI-FAC is proposed. In the end, the activation energy (Ea) of Pd3.75Ag3.75-PEI-FAC catalyst is calculated to 53.97 kJ mol-1, and this catalyst shows unique robustness and satisfactory re-usability with no loss of catalytic activity after five recycles. The findings in this work provide a novel routine from lignocellulose fractionation towards cellulose-derived catalyst for H2 evolution. 相似文献
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Abdul Ghaffar Masaaki Tabata Farhana Mazher Azhar Mashiatullah 《Environmental Chemistry Letters》2012,10(2):171-176
This article reports high dechlorination of toxic polychlorinated biphenyls (PCBs) under mild conditions. PCBs are priority
pollutants acting as endocrine disruptors, human carcinogens and environmental estrogens. Previous remediation methods involving
high temperature and pressure have drawbacks such as high cost, de novo dioxins synthesis and difficult recovery of vaporized
PCBs. On the other hand, dechlorination methods using mild conditions show the problem of catalyst deactivation. Here, activated
carbon was used for the first time as catalyst to dechlorinate 2,4,5 trichlorobiphenyl. High dechlorination, of 87%, was achieved
under mild conditions. 2,4,5 trichlorobiphenyl was treated at 40–150°C with calcium hydroxide, sodium hydroxide and sulfur
in mixed water and organic solvents. Dechlorination products were biphenyl, orthohydroxy biphenyls, 2,4 dihydroxy biphenyls
and biphenyl-2-thiol. Dichlorobiphenyl and orthochlorobiphenyls were found in trace quantities. We found that carbon particles
catalysed dechlorination by substitution reactions and suppressed further chlorination. Dechlorination at biphenyl ortho position
was preceded by substitution reaction by hydroxyl and thiol ions. Moreover, in the absence of carbon, dechlorination was lower
and substituted products were not observed. These findings may be applied at industrial scale to remediate PCB-contaminated
waste. 相似文献