Ghauch Antoine, Tuqan Almuthanna
American University of Beirut, Faculty of Arts and Sciences, Department of Chemistry, Beirut, Lebanon.
Chemosphere. 2008 Oct;73(5):751-9. doi: 10.1016/j.chemosphere.2008.06.035.
Modified zero valent iron (MZVI) was used to study the transformation of a chlorothalonil (CLT) solution and the variation of the observed degradation rate of the reduction reactions. This was carried out when transition metals e.g. Pd, Cu and Co plated on the surface of micrometric iron particles (< 150 microm) were used as reducing catalytic agents for pesticide removal. Reactions were undertaken under both oxic and anoxic conditions in the presence and the absence of a phosphate buffer solution (PBS). Results of batch studies in nitrogen sparged solutions revealed that incomplete slow dechlorination merely occurred with zero valent iron (ZVI), however, complete rapid dechlorination reactions took place with MZVI especially Fe/Pd. Dechlorination was depicted by studying UV absorbance and MS spectra of CLT and all corresponding by-products. Typical blue shifts (deltalambda = 4-6 nm/chlorine atom) were observed at the same time as chlorine cluster isotopes disappeared. After the plating process, metal loading was controlled by analyzing the remaining metal in the solution by atomic absorption spectroscopy. Experiments showed that CLT degradation mechanism is faster in nitrogen sparged solutions in the absence of PBS. Time needed for complete removal of 2.08 +/- 0.19 microM CLT solution was about 2 h when experiments were conducted with ZVI (t1/2 = 15.0 min) and about 10 min when the reaction was carried out under the same conditions with Fe/Pd 1% (t1/2 = 1.0 min). Degradation rates for all bimetallic systems were determined showing that Pd is the more exciting catalytic transition metal followed by Cu and Co. Furthermore, MZVI method showed obvious advantage to traditional CLT treatment methods.
采用改性零价铁(MZVI)研究百菌清(CLT)溶液的转化以及还原反应中观察到的降解速率变化。当镀在微米级铁颗粒(<150微米)表面的过渡金属如钯、铜和钴用作去除农药的还原催化剂时进行了此项研究。反应在有氧和无氧条件下,分别在有和没有磷酸盐缓冲溶液(PBS)的情况下进行。在氮气鼓泡溶液中的批次研究结果表明,零价铁(ZVI)仅发生不完全的缓慢脱氯反应,然而,MZVI尤其是Fe/Pd发生了完全快速的脱氯反应。通过研究CLT及其所有相应副产物的紫外吸光度和质谱来描述脱氯过程。在氯簇同位素消失的同时观察到典型的蓝移(Δλ = 4 - 6 nm/氯原子)。镀覆过程后,通过原子吸收光谱分析溶液中剩余的金属来控制金属负载量。实验表明,在没有PBS的氮气鼓泡溶液中,CLT的降解机制更快。用ZVI进行实验时,完全去除2.08±0.19 microM CLT溶液所需的时间约为2小时(t1/2 = 15.0分钟),而在相同条件下用1%的Fe/Pd进行反应时约为10分钟(t1/2 = 1.0分钟)。测定了所有双金属体系的降解速率,结果表明钯是更具活性的催化过渡金属,其次是铜和钴。此外,MZVI方法对传统的CLT处理方法显示出明显优势。