Continuous rapid dechlorination of p-chlorophenol by Fe-Pd nanoparticles promoted by procyanidin
Continuous rapid dechlorination of p-chlorophenol by Fe-Pd nanoparticles promoted by procyanidin
复制标题
原花青素促进 Fe-Pd 纳米粒子连续快速脱氯对氯苯酚
DOI：
10.1016/j.ces.2019.02.024
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发表时间：
2019-06-29
影响因子：
4.7
通讯作者：
He, Zhimin
中科院分区：
文献类型：
--
作者：
Liu, Mingyue;Huan, Renliang;He, Zhimin
纳米零价铁在环境修复和有毒废物处理中有着广泛的应用，尤其是在持久性有机污染物（POPs）的降解方面。然而，铁纳米粒子（铁NPs）的脱氯活性可以抑制铁钯NPs在碱性条件下的腐蚀产生的铁氧化物的沉淀，导致脱氯效率降低。面对这一挑战，我们报告了一种高效的脱氯系统，该系统在广泛的pH值范围内发挥作用，特别是在碱性条件下。原花青素（PROC），一种天然多酚，被用作稳定剂，以操纵Fe-Pd纳米颗粒的尺寸分布，更重要的是，作为铁离子的清除剂，以防止氧化铁沉淀。实验和理论计算表明，生成的Fe离子主要以双和三PROC-Fe络合物的形式存在于反应溶液中。与原始的Fe-Pd纳米颗粒相比，经修饰的Fe-Pd纳米颗粒的脱氯效率提高了20倍（pH 9.0）。值得注意的是，归一化速率常数提高了2个数量级以上，以前报道的脱氯系统。在较宽的pH值范围内（2.3 - 13.0），改性后的Fe-Pd纳米粒子表现出优异的脱氯效率。(C)2019爱思唯尔有限公司版权所有。
Nanoscale zero-valent iron has been widely applied in environmental remediation and toxic waste treatment, especially for the degradation of persistent organic pollutants (POPs). However, the dechlorination activity of Fe nanoparticles (Fe NPs) can be suppressed by the precipitation of iron oxides generated from the corrosion of Fe-Pd NPs under alkaline conditions, leading to a decreased dechlorination efficiency. Faced with this challenge, we report a highly effective dechlorination system that functions over a broad pH range and especially well under alkaline conditions in this work. Procyanidin (PROC), a natural polyphenol, was utilized as a stabilizer to manipulate the size distribution of Fe-Pd NPs and, more importantly, as a scavenger of Fe ions to prevent iron oxide precipitation. Experiments and theoretical calculations reveal that the generated Fe ions was mainly present in the form of bis- and tris-PROC-Fe complexes in the reaction solution. Compared with pristine Fe-Pd NPs, the PROC-modified Fe-Pd NPs had a dechlorination efficiency that was increased 20-fold (pH 9.0). Notably, a normalized rate constant was enhanced by more than 2 orders of magnitude compared to the previously reported dechlorination systems. The PROC-modified Fe-Pd NPs showed excellent dechlorination efficiency over a wide pH range (2.3-13.0). (C) 2019 Elsevier Ltd. All rights reserved.