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標題: Effects of interference resistance by chloride and total basicity capacity of surface on aqueous Hg(II) adsorption by multi-walled carbon nanotubes
作者: 許振&#23791
Cheng-Feng Hsu
關鍵字: 汞;奈米碳管;吸附作用;氯離子;動力吸附;等溫吸附;總鹼基含量;mercury;multi-walled carbon nanotubes;adsorption;chloride;isotherm;kinetics;total basicity capacity.
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本研究探討多壁奈米碳管 (multi-walled carbon nanotubes, MWCNTs) 表面總鹼基含量及水中Cl-Hg物種隨不同氯離子濃度與pH變化下,對MWCNTs吸附水中二價汞 (Hg(II)) 之影響。經研究結果顯示,水中氯離子濃度越高 (> 0.01 M),Hg(II)去除率越低;而Hg(II)去除率隨pH增加之變化,主要受:(1)水中質子(H+)與Hg(II)競爭表面鹼性位址、(2)中性HgCl2及Hg(OH)2取代正電荷Hg2+及HgOH+與(3)表面負電荷斥力與物理性吸附力之交互影響。
經評估不同動力模式之模擬值與實驗值,皆具有pseudo-second- order model、intraparticle diffusion model及Elovich model之特性;而在等溫吸附實驗方面,以OH-MWCNT於pH = 4.3條件下有最高之實驗飽和吸附容量89.42 mg/g,並以Freundlich model模擬結果較吻合MWCNTs異質性表面;另外含有–COOH及–OH官能基的MWCNTs,雖然增加MWCNTs親水性而有助於對Hg(II)的吸附,但主要是改質後MWCNTs之表面總鹼基含量提高,使Hg(II)去除率提高,顯示還原特性對提高Hg(II)吸附量有正面之影響,但經吸附平衡再脫附游離於水中的殘留Hg則不易再被吸附,推測是部分Hg(II)被還原為Hg(I)物種,降低與MWCNTs之親和力。故MWCNTs吸附Hg(II)有多樣性吸附特徵,其吸附反應路徑主要為還原反應與凡得瓦爾力,次要為離子交換機制與氫鍵作用力,此特性使得MWCNTs在環境污染整治之應用,對含汞污染之水體處理具有開發應用之潛能,仍是未來應持續開發的新興科技。

This study evaluated the interference resistance effects of chloride and total basicity capacity on inorganic divalent mercury (Hg(II)) adsorption by modified multi-walled carbon nanotubes (MWCNTs) in various pH values. The results revealed that the adsorption capacity of Hg(II) was decreasing by both increase of pH value and the ionic strength (the range of chloride ion from 0 to 1.0 mol/L). Those phenomena could be critically determined by: (1) the competition between proton (H+) and Hg(II) on empty adsorption base sites; (2) Hg2+ and HgOH+ in place of neutral species of HgCl2 and Hg(OH)2; (3) the surface interaction between negative repulsive force and physisorption.
The results from a kinetic investigation demonstrated that the adsorption of Hg(II) by MWCNTs could be partially described by three kinetic models, the pseudo-second-order model, intraparticle diffusion model, and Elovich model, respectively. Additionally, the kinetic results also indicated that the adsorption of Hg(II) by MWCNTs was significantly affected by chemical adsorption characteristics and the heterogeneous surface sites. The Freundlich isotherm was provided the appropriate illustration in the equilibrium adsorption for adsorption of Hg(II) by MWCNTs. The maximum adsorption capacity of Hg (II) by OH-MWCNT was 89.72 mg/g at the pH value of 4.3, indicating the function of features by heterogeneous surface sites of MWCNTs is the major mechanism during the adsorption process. Additionally, the adsorption capacity was significant increased with increasing hydrophilicity of MWCNT, which derived from –COOH and –OH functional groups of MWCNTs. However, the total basicity capacity was the mean role for Hg(II) adsorption. The results of adsorption isotherm and kinetic also indicated that the adsorption performance of Hg(II) was in proportion to the reductive reaction. Furthermore, we found out the remaining mercury compounds when the adsorption reached to equilibrium that caused Hg(II) would be difficult to re-adsorbed, which might be deduced by the partial Hg(II) species reduced to Hg(I) in residual aqueous solution to decrease the affinity on MWCNTs.
Consequently, the study outcomes were conducted to evaluate the characteristics of Hg(II) adsorption by MWCNTs as an multiple pattern. The predominant reaction pathways of adsorption Hg(II) were followed up the reduction reaction and van der Waals forces. However, the ion exchange and hydrogen bonding were minor during adsorption procedure. The results obtained are potentially application MWCNTs for removal of Hg(II) in the remediation of environmental contamination and deserved be explored continually.
其他識別: U0005-2206201523151000
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