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首页> 外文期刊>Separation and Purification Technology >Catalytic hydrodechlorination of chlorophenols by Pd/Fe nanoparticles: Comparisons with other bimetallic systems, kinetics and mechanism
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Catalytic hydrodechlorination of chlorophenols by Pd/Fe nanoparticles: Comparisons with other bimetallic systems, kinetics and mechanism

机译：Pd / Fe纳米粒子对氯酚的催化加氢脱氯：与其他双金属体系的比较，动力学和机理

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摘要

This study investigated dechlorination of 4-chlorophenol (4CP), 2,4-dichlorophenol (24DCP), and 2,4,6-trichlorophenol (246TCP) with Pd/Fe nanoparticles. The reaction rates were significantly faster than those achieved with Pt/Fe, Ni/Fe, Cu/Fe and Co/Fe nanoparticles. The chlorophenols (CPs) could be completely reduced to phenol by Pd/Fe following the pseudo-first-order kinetics, and the rates followed the order of 246TCP < 24DCP < 4CP. The 246TCP reduction rate with Pd/Fe increased with temperature and the estimated activation energy was 29.8 kj/mol. The CPs dechlorination rate increased linearly with Pd loading, suggesting that Pd catalyst could be the only reactive site. Based on rigorous analysis of the transient formations and concentrations of various intermediates, a scheme of transformation pathways and the reaction mechanism was proposed to delineate 246TCP dechlorination to phenol. The influence of pH on the CPs dechlorination was investigated, and weak acidic condition is more favorable to the dechlorination reaction. H2 evolution or iron corrosion rate initially followed the pseudo-first-order kinetics, and was reverted to the zero-order kinetics for prolonged reaction (>24h).
机译：这项研究研究了Pd / Fe纳米粒子对4-氯苯酚（4CP），2,4-二氯苯酚（24DCP）和2,4,6-三氯苯酚（246TCP）的脱氯作用。反应速率明显高于使用Pt / Fe，Ni / Fe，Cu / Fe和Co / Fe纳米颗粒所达到的速度。遵循伪一级动力学原理，Pd / Fe可以将氯酚（CPs）完全还原为苯酚，其速率遵循246TCP <24DCP <4CP的顺序。 Pd / Fe的246TCP还原速率随温度增加而增加，估计的活化能为29.8 kj / mol。 CPs的脱氯速率随Pd的添加呈线性增加，表明Pd催化剂可能是唯一的反应中心。在对各种中间体的瞬时形成和浓度进行严格分析的基础上，提出了将246TCP脱氯描述为苯酚的转化途径和反应机理。研究了pH对CPs脱氯的影响，弱酸性条件更有利于脱氯反应。 H2的析出或铁腐蚀速率最初遵循拟一级动力学，然后恢复为零级动力学以延长反应时间（> 24h）。

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