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標題: 不同粒徑針鐵礦影響六價鉻吸附與光催化還原反應
The effects of particle sizes of goethite on the adsorption and photocatalytic reduction of Cr(VI)
作者: 吳秉學
Wu, Pin-Hsueh
關鍵字: 針鐵礦;goethite;六價鉻;粒徑;吸附;光催化;Cr(VI);particle size;adsorption;photocatalytic reduction
出版社: 土壤環境科學系所
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本研究主要探討不同粒徑之針鐵礦與環境中的毒性陰離子六價鉻之交互作用。針鐵礦的製備採用ferrihydrite熱轉變法、硝酸鐵酸式法和硫酸鐵法分別合成22、139和449 nm三種不同粒徑針鐵礦,另外也以Schwertmann合成法來進行較大粒徑的針鐵礦(849和1207 nm)。合成的針鐵礦樣品利用雷射粒徑儀分析和穿透顯微鏡(TEM)觀測其粒徑及外部型態,以X光粉末繞射儀(XRD)鑑定針鐵礦結晶,以及利用BET比表面積儀和等電位點(ZPC)儀器量測各種粒徑之表面積和表面電位。不同粒徑之針鐵礦對六價鉻的吸附,分別符合Elovich動力模式和Langmuir等溫模式,針鐵礦對六價鉻的吸附量(qmon)介於0.0707-0.207 mmol/g之間,隨針鐵礦粒徑大小之降低而增加,此增加與比表面積之大小有關且其與粒徑大小呈線性關係。隨pH值升高,各粒徑之針鐵礦對六價鉻的吸附均在pH 6-8間有明顯的下降,此與六價鉻之物種轉變為CrO42-或與針鐵礦表面負電荷及氫氧離子之增加有關。針鐵礦對六價鉻的吸附熱隨粒徑之降低而增高,此可能與被吸附的六價鉻從小粒徑針鐵礦的脫附能力較低有關。小粒徑針鐵礦對六價鉻催化還原為三價鉻的能力較高,此可能與小粒徑針鐵礦對六價鉻的吸附能力高,且電子在其表面轉移的能力較快有關。

This study mainly investigates the interactions of Cr(VI), a toxic anion in the environment, with goethite with different particle sizes. Several methods were used for goethite syntheses, including ferrihydrite heat transformation, ferric nitrate acidification, and ferric sulfate, which gave particle sizes of 22, 139, and 449 nm, respectively. In addition, a method adopted from Schwertmanm was employed for preparing goethite with greater particle sizes of 849 and 1207 nm. The results of powder X-ray diffraction (XRD) conformed the goethite structures for each synthesized samples. The particle sizes and morphologies of these goethite samples were further verified using a laser scattering particle size distribution analyzer and a transmission electron microscopy (TEM). Surface areas and pHzpc (zero point charge) for each particle were measured using a BET surface area meter and Zeta meter. Cr(VI) adsorption on goethite complied with Elovich kinetic model and Langmuir adsorption isotherm, and the adsorption behaviors was indifferent with the particle sizes of goethite. The maximum adsorption of Cr(VI) on goethite was in the range 0.0707-0.207 mmol/g, depending on the particle size of goethite. A liner relationship existed between the amount of Cr(VI) adsorption and the goethite particle sizes and the smaller goethite particle exhibited higher adsorption ability, corresponding to its higher surface area. A significant declination of Cr(VI) adsorption on goethite was observed at pH 6-8, related probably to the change in Cr(VI) species (i.e., converting from HCrO4- to CrO42- at the specific pH) or/and an increase of surface negative charges and OH ion concentrations. An apparent endothermic reaction was observed while adsorbing Cr(VI) on goethite. Cr(VI) adsorption on smaller particle size of goethite had higher absorption heat which may lead to a decrease of Cr(VI) desorption from the surfaces of small particles. Small particles revealed a higher efficiency for photo-catalytic reduction of Cr(VI) on goethite, attributing to the higher adsorption ability of Cr(VI) and rapid electric transferring on the surfaces of small goethite particles.
其他識別: U0005-1608201211071900
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