Please use this identifier to cite or link to this item: http://hdl.handle.net/11455/28152
標題: 奈米零價鐵鈀還原降解五氯酚之研究
Reduction of Pentachlorophenol by Nanoscale Pd0/Fe0 Bimetallic Particles
作者: 陳孟宜
Chen, Meng-Yi
關鍵字: pentachlorophenol
五氯酚
nanoscale Palladium/iron
degradation
奈米零價鐵鈀
降解
出版社: 土壤環境科學系所
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摘要: Pentachlorophenol (PCP), one of persistent organic pollutant (POP) and also a carcinogenic compound, has been used widely as wood preservative and pesticides in the past. Due to the improper storage and disposal of these persistent organic pollutants, several POP contaminated sites were found in the world, especially a PCP contaminated site in Taiwan. Nanoscale zerovalent metal particles were developed to in-situ chemically degrade poly-halogenated aromatic contaminants. Nanoscale Pd0/Fe0 particles we synthesized were used to evaluate the potential of Pd0/Fe0 nanoparticles for the remediation the PCP contaminated sites. The effects of nanoscale Pd0/Fe0 dosage, palladium loading, PCP concentrations, and aqueous parameters such as different concentration of various common cations and anions, temperature, and pH, on the degradation of PCP were performed. And the removal experiments of PCP in PCP contaminated soil and Lukang soil were investigated. The increase of nanoscale Pd0/Fe0 dosage results in the increase in PCP degradation rate and efficiency due to more Pd0/Fe0 surface to reduce PCP. With the increase of the palladium loading percentage from 0.02 wt % to 0.054 wt %, PCP degradation rates increased but the degradation rate slightly decreased with the increase of the palladium loading percentage from 0.054 wt % to 0.13 wt %. It seems a common characteristic for catalyst. The effect of initial PCP concentrations on the removal rate can be described by a surface kinetic model, Langmuir-Hinshelwood model. The estimated activation energy of the dechlorination reactions of 29 kJ/mol indicates that the degradation of PCP on Pd0/Fe0 nanoparticle is a surface-control mechanism. The effects of common cations and anions on the degradation of PCP with Pd0/Fe0 nanoparticles were needed to be studied. Common groundwater anions inhibited PCP reduction in increasing order of Cl- < HCO3- < SO42- < HPO42- < NO3-, which is generally consistent with their affinity to form complexes with iron oxide except NO3- and HCO3-. Generally, the inhibition effect increased with the increase of anion concentrations. Nitrate may compete electrons offered from iron with PCP to reduce other nitrogen species. The smallest pH variation before and after experiments indicates that HCO3- has pH buffer capacity. In the presence of sulfate, which can cause for inhibition, cation Na+ was proposed to have no influence the degradation efficiencies of PCP and used as a reference. Cations Mg2+, Cu2+, Ni2+ and Fe3+ could facilitate the degradation efficiencies of PCP with nanoscale Pd0/Fe0 particles in increasing order of Cu2+ < Mg2+ < Fe3+ < Ni2+. With chloride ions, the smallest effect in our anions, the decrease trend of PCP degradation for these cations is similar, except Cu2+. Moreover, Ni2+ could increase the degradation kinetics and efficiency of PCP with Pd0/Fe0 nano-particles although either sulfate or chloride ions inhibit the degradation behaviors. The increase of concentration of soil solution showed a negative effect on the degradation rate constants of PCP by nanoscale Pd0/Fe0 particles. Soil solution containing common anions may inhibit the degradation. The anions in soil solutions would form iron-complex or metal oxides precipitation on nanoscale Pd0/Fe0 particles to decrease the surface reactivity. According to the instant occurrence of degraded byproducts, tetrachlorophenols, trichlorophenols, dichlorophenols, chlorophenols, and phenol during the reaction, multiple dechlorination process is proposed for the PCP degradation reaction on the nanoscale Pd0/Fe0 particles. The chlorine atom at the ortho and meta positions can be more easily dechlorinated than that at para position on PCP. It results from the steric effect of chloride on PCP structure. An efficient degradation of the PCP with nanoscale Pd0/Fe0 particles in soils was performed in this study. The degradation efficiency and kinetics of PCP in Lukang soil are less than these in PCP contaminated soil due to the higher nitrate concentration and higher soil organic carbon in Lukang soil than PCP contaminated soil. Nitrate ions inhibit the reduction of PCP. The low degradation efficiency could also result from larger adsorption of PCP in Lukang soil. The colloids in soils may also decrease the degradation efficiency in the application of removal of PCP with nanoscale Pd0/Fe0 particles so a higher amount of Pd/Fe nanoparticles was used in soil than in solution. These better understandings can facilitate the remediation design and the prediction of treatment efficiency of PCP with nanoscale Pd0/Fe0 particles. Nanoscale Pd0/Fe0 particles could be a potential remediation agent for PCP contaminated sites because their rapid removal reactions of PCP occur in soils and groundwater and an excess of the nanoscale Pd0/Fe0 particles in the soils can provide an extra reducing power to reduce the target polyhalogenated aromatic compounds of PCP.
五氯酚 (pentachlorophenol, PCP) 過去使用於木材保護劑與殺蟲劑,其為持久性之有機污染物 (persistent organic pollutants, POP) 且具致癌性。由於不適當儲存與廢棄這些持久性有機污染物,世界已有許多POP污染場址,台灣已發現PCP污染場址。而奈米零價鐵鈀 (palladium/iron, Pd0/Fe0) 顆粒之技術已發展於現地化學還原含鹵素有機污染物。 此研究以批次實驗系統應用自行合成之奈米Pd0/Fe0移除PCP,評估以供復育污染場址之潛力。由於增加奈米Pd0/Fe0劑量使其具較多之Pd0/Fe0表面以還原PCP,故其降解速率提高。奈米Pd0/Fe0顆粒之Pd重量百分比於0.02 wt %至0.054 wt %之間,則增加Pd重量百分比則會提高PCP之降解速率,但若增加Pd之重量百分比至 0.13 wt %,則會降低PCP之降解速率。PCP初始濃度之影響可以Langmuir-Hinshelwood模式描述,另外經計算求得之活化能為29 kJ/mol,此結果顯示利用奈米Pd0/Fe0降解PCP為一表面控制反應。 地下水中常見之陰離子會抑制PCP之降解效率,其抑制的順序依序為Cl- < HCO3- < SO42- < HPO42- < NO3-。除了NO3-與HCO3-之外,此抑制順序與這些陰離子與鐵氧化物產生複合物之親合力順序相符,抑制程度隨其濃度增加而增加。而NO3-會與PCP競爭電子而使其還原成其他含氮化合物,所以抑制PCP之降解效率最顯著。HCO3-因其具有pH緩衝能力而減少抑制PCP之降解效率。 在SO42-為背景陰離子之情況下,因如前所述,SO42-會抑制奈米Pd0/Fe0降解PCP,又因Na+之高還原電位,所以Na+應不影響奈米Pd0/Fe0降解PCP,可作為比較之基準。所以相較於相同濃度之下,Mg2+、Cu2+、Ni2+與Fe3+則可促進PCP之降解效率,其促進之順序依序為Cu2+ < Mg2+ < Fe3+ < Ni2+。此外,Ni2+即使未扣除SO42-之影響,其亦會促進PCP之降解效率。而在以Cl-為背景陰離子之情況下,相同地以Cl-為抑制奈米Pd0/Fe0降解PCP之原因,所以NaCl對利用奈米Pd0/Fe0降解PCP的影響作為比較基準。Mg2+、Ni2+與Fe3+則可促進PCP之降解效率,其促進之順序依序為Mg2+ < Fe3+ < Ni2+。但Cu2+會抑制PCP之降解效率。此外,Ni2+即使未扣除Cl-之影響,其亦會促進PCP之降解效率。 於土壤溶液方面,增加鹿港系土壤溶液之濃度則會降低PCP之降解速率。由於土壤溶液中含不同陰陽離子,土壤溶液中之陰離子會與鐵形成鐵複合物而於奈米Pd0/Fe0顆粒上產生礦物沉澱,進而降低其表面活性而降低反應奈米Pd0/Fe0之降解效率。 在反應過程中偵測到四氯酚、三氯酚、二氯酚、氯酚以及酚為其副產物,推測降解反應為多步降解過程。奈米Pd0/Fe0於PCP之鄰位(othro)及間位(meta)取代基之脫氯作用較對位(para)取代基多,原因為移除PCP之氯取代基位置取決於減少PCP之立體結構障礙。 本研究亦有效地降解鹿港系土壤與PCP污染土壤中之PCP,PCP於鹿港系土壤中之降解速率較於PCP污染土壤中之降解速率低。由於鹿港系土壤中之NO3-濃度較PCP污染土壤中高而抑制PCP之還原。土壤中之碳含量百分比亦會影響PCP之降解速率,因碳含量百分比高之土壤增加PCP於土壤之吸附作用而抑制奈米Pd0/Fe0降解PCP。而鹿港系土壤之碳含量百分比較PCP污染土壤高,故其會降低PCP降解速率。而另外,土壤膠體亦會影響奈米Pd0/Fe0於土壤中降解PCP之應用。 此結果可更加了解利用奈米Pd0/Fe0降解PCP污染場址復育之設計方式與預期其處理效果。由於奈米Pd0/Fe0具快速還原PCP之能力,故利用其降解PCP可作為整治PCP污染場址之有效方式。
URI: http://hdl.handle.net/11455/28152
其他識別: U0005-2512200815104000
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