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金掺杂生物 Pd 催化剂可在环境条件下使双氯芬酸脱氯。

Doping of biogenic Pd catalysts with Au enables dechlorination of diclofenac at environmental conditions.

机构信息

Laboratory of Microbial Ecology and Technology (LabMET), Ghent University, Coupure Links 653, B-9000 Gent, Belgium.

出版信息

Water Res. 2012 May 15;46(8):2718-26. doi: 10.1016/j.watres.2012.02.036. Epub 2012 Feb 24.

Abstract

By using the metal reducing capacities of bacteria, Pd nanoparticles can be produced in a sustainable way ('bio-Pd'). These bio-Pd nanoparticles can be used as a catalyst in, for example, dehalogenation reactions. However, some halogenated compounds are not efficiently degraded using a bio-Pd catalyst. This study shows that the activity of bio-Pd can be improved by doping with Au(0) ('bio-Pd/Au'). In contrast with bio-Pd, bio-Pd/Au could perform the removal of the model pharmaceutical compound diclofenac from an aqueous medium in batch experiments at neutral pH and with H(2) as the hydrogen donor (first order decay constant of 0.078 ± 0.009 h(-1)). Dehalogenation was for both catalysts the only observed reaction. For bio-Pd/Au, a disproportional increase of catalytic activity was observed with increasing Pd-content of the catalyst. In contrast, when varying the Au-content of the catalyst, a Pd/Au mass ratio of 50/1 showed the highest catalytic activity (first order decay value of 0.52 ± 0.02 h(-1)). The removal of 6.40 μg L(-1) diclofenac from a wastewater treatment plant effluent using bio-Pd was not possible even after prolonged reaction time. However, by using the most active bio-Pd/Au catalyst, 43.8 ± 0.5% of the initially present diclofenac could be removed after 24 h. This study shows that doping of bio-Pd nanoparticles with Au(0) can be a promising approach for the reductive treatment of wastewaters containing halogenated contaminants.

摘要

利用细菌的金属还原能力,可以以可持续的方式生产钯纳米粒子(“生物-Pd”)。这些生物-Pd 纳米粒子可用作催化剂,例如在脱卤反应中。然而,一些卤代化合物不能有效地用生物-Pd 催化剂降解。本研究表明,通过掺杂 Au(0)(“生物-Pd/Au”)可以提高生物-Pd 的活性。与生物-Pd 相比,生物-Pd/Au 可以在中性 pH 值和 H 2 作为氢供体的间歇实验中从水介质中去除模型药物化合物双氯芬酸(一级衰减常数为 0.078 ± 0.009 h -1)。对于两种催化剂,脱卤都是唯一观察到的反应。对于生物-Pd/Au,随着催化剂中 Pd 含量的增加,催化活性呈不成比例的增加。相比之下,当改变催化剂中的 Au 含量时,催化剂中 Pd/Au 的质量比为 50/1 时表现出最高的催化活性(一级衰减值为 0.52 ± 0.02 h -1)。即使延长反应时间,使用生物-Pd 也无法从污水处理厂废水中去除 6.40 μg L -1 的双氯芬酸。然而,使用最活跃的生物-Pd/Au 催化剂,在 24 h 后可以去除初始存在的双氯芬酸的 43.8 ± 0.5%。本研究表明,用 Au(0)掺杂生物-Pd 纳米粒子可能是处理含有卤代污染物的废水的一种很有前途的方法。

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