可回收纳米钯工程天然海绵与甲酸催化三种有机氯的脱氯作用

Catalysts Pub Date : 2024-07-03 DOI:10.3390/catal14070424
Mingyue Liu, Gang Chen, Zhenjun Song, Zhicai He, Aiguo Zhong, Mei Cui
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引用次数: 0

摘要

钯(Pd)与 HCOOH 催化有机氯化物脱氯是最有效、最有前景的环境修复技术之一。本研究采用碱性改性多孔天然海绵作为 Pd 纳米催化剂(Pd@M-Sponge)的载体,以 HCOOH 作为氢源,对氟苯尼考(FF)、邻氯苯酚(o-CP)和对氯苯酚(p-CP)进行加氢脱氯。在 25 °C、常压条件下,FF、邻氯苯酚和对氯苯酚实现了良好的转化效率,这归功于制备的 Pd NPs 直径小、催化反应活性高,以及制备的 Pd@M-Sponge 有轻微的内部传质限制。即使在 HCOOH 与对氯化石蜡的摩尔比很低(10:1)和对氯化石蜡浓度很高(500 mg/L)的条件下,也能获得很高的反应速率常数。所制备的催化剂还具有优异的可回收性,在 20 个连续的对氯联苯脱氯循环中,催化反应活性没有明显下降。这项工作为甲酸催化加氢脱氯氯化有机污染物提供了一种基于可再生和生物相容性天然材料的理想的可回收和具有成本效益的催化剂,也为探索和设计高活性和高稳定性的加氢脱氯催化剂提供了新的视角。
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Catalytic Dechlorination of Three Organochlorides by Recyclable Nano-Palladium-Engineered Natural Sponge with Formic Acid
Catalytic dechlorination of organic chlorides by palladium (Pd) with HCOOH represents one of the most effective and promising techniques for environmental remediation. In this study, we adopted alkaline-modified porous natural sponge as support of a Pd nanocatalyst (Pd@M-Sponge) and HCOOH as a hydrogen source for the hydrodechlorination of florfenicol (FF), o-chlorophenol (o-CP), and p-chlorophenol (p-CP). Favorable conversion efficiency of FF, o-CP, and p-CP was achieved at 25 °C and atmospheric pressure attributed to the small diameter and high catalytic reactivity of the prepared Pd NPs, in addition to the slight internal mass transfer limitation of the prepared Pd@M-Sponge. High reaction rate constants were obtained even in the conditions of a low molar ratio of HCOOH to p-CP (10:1) and a high concentration of p-CP (500 mg/L). The prepared catalyst also demonstrated superior recyclability without any obvious decrease in catalytic reactivity in 20 successive p-CP dechlorination cycles. This work provides an ideal recyclable and cost-effective catalyst based on renewable and biocompatible natural material for the catalytic hydrodechlorination of chlorinated organic pollutants with formic acid and a new view for the exploration and designing of highly reactive and stable catalysts for hydrodechlorination.
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