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Catalytic hydrodechlorination of triclosan using a new class of anion-exchange-resin supported palladium catalysts

机译:新型阴离子交换树脂负载钯催化剂催化三氯生加氢脱氯

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We prepared a new class of anion-exchange-resin supported Pd catalysts for efficient hydrodechlorination of triclosan in water. The catalysts were prepared through an initial ion-exchange uptake of PdCl42- and subsequent reduction of Pd(II) to Pd(0) nanoparticles at ambient temperature. Two standard strong-base anion exchange resins (IRA-900 and IRA-958) with different matrices (polystyrene and polyacrylic) were chosen as the supports. SEM and TEM images showed that Pd(0) nanoparticles were evenly attached on the resin surface with a mean size of 3-5 nm. The resin supported Pd catalysts (Pd@IRA-900 and Pd@IRA-958) were able to facilitate rapid and complete hydrodechlorination of triclosan. At a Pd loading of 2.0 wt.%, the observed pseudo first-order rate constant (k(obs)) was 1.25 +/- 0.06 and 1.6 +/- 0.1 L/g/min for Pd@IRA-900 and Pd@IRA-958, respectively. The catalysts were more resistant to Cl- poisoning and natural organic matter fouling than other supported-Pd catalysts. The presence of 10 mM NaCl suppressed the kobs value by 31% and 23% for Pd@IRA-900 and Pd@IRA-958, whereas the presence of humic acid at 30 mg/L as TOC lowered the rates by 28% and 27%, respectively. The better performance of Pd@IRA-958 was attributed to the polymeric matrix properties (i.e., hydrophobicity, pore size, and surface area) as well as Pd particle size. GC/MS analyses indicated that very low concentrations of chlorinated intermediates were detected in the early stage of the hydrodechlorination process, with 2-phenoxyphenol being the main byproduct. The catalysts can be repeatedly used in multiple operations without significant bleeding. The catalysts eliminate the need for calcination in preparing conventional supported catalysts, and the resin supports conveniently facilitate control of Pd loading and material properties. (C) 2017 Elsevier Ltd. All rights reserved.
机译:我们制备了一类新型的阴离子交换树脂负载的Pd催化剂,用于水中三氯生的有效加氢脱氯。通过在室温下初始吸收PdCl42-进行离子交换,然后将Pd(II)还原为Pd(0)纳米粒子来制备催化剂。选择两种具有不同基质(聚苯乙烯和聚丙烯酸酯)的标准强碱阴离子交换树脂(IRA-900和IRA-958)作为载体。 SEM和TEM图像显示Pd(0)纳米颗粒均匀附着在树脂表面,平均尺寸为3-5 nm。树脂负载的Pd催化剂(Pd @ IRA-900和Pd @ IRA-958)能够促进三氯生的快速和完全加氢脱氯。在Pd含量为2.0 wt。%时,对于Pd @ IRA-900和Pd @,观察到的拟一级反应速率常数(k(obs))为1.25 +/- 0.06和1.6 +/- 0.1 L / g / min分别是IRA-958。与其他负载型钯催化剂相比,该催化剂对氯中毒和天然有机物结垢的抵抗力更高。 10 mM NaCl的存在将Pd @ IRA-900和Pd @ IRA-958的kobs值抑制了31%和23%,而30 mg / L的腐殖酸的TOC降低了28%和27的腐殖酸发生率。 %, 分别。 Pd @ IRA-958的更好性能归因于聚合物基质的性能(即疏水性,孔径和表面积)以及Pd粒径。 GC / MS分析表明,在加氢脱氯过程的早期阶段,检测到非常低浓度的氯化中间体,其中2-苯氧基苯酚是主要副产物。催化剂可以重复使用多次,而不会产生明显的渗色。该催化剂消除了制备常规负载型催化剂中煅烧的需要,并且树脂载体方便地促进了Pd负载量和材料性能的控制。 (C)2017 Elsevier Ltd.保留所有权利。

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