The consortium of heterogeneous cobalt phthalocyanine catalyst and bicarbonate ion as a novel platform for contaminants elimination based on peroxymonosulfate activation
The consortium of heterogeneous cobalt phthalocyanine catalyst and bicarbonate ion as a novel platform for contaminants elimination based on peroxymonosulfate activation
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多相钴酞菁催化剂和碳酸氢根离子的联合体作为基于过一硫酸盐活化的污染物消除新平台
DOI：
10.1016/j.jhazmat.2015.08.063
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发表时间：
2016-01-15
影响因子：
13.6
通讯作者：
Chen, Wenxing
中科院分区：
文献类型：
--
作者：
Huang, Zhenfu;Yao, Yuyuan;Chen, Wenxing
高效催化氧化工艺的设计长期以来一直是环境催化领域的研究热点。在本工作中，将纤维素纤维键合的钴酞菁(CFS-COPC)与过氧单硫酸盐(PMS)偶联，形成了一种新型的氧化体系CFS-COPC/PMS。CFS-COPC/PMS体系在35min内对酸性红1(AR1)等偶氮染料的脱色率接近100%，是一种高效的氧化过程。此外，还进一步将碳酸氢根离子(HCO3-)引入到CFS-COPC/PMS中，构建了CFS-COPC/PMS/HCO3-复合体系。值得注意的是，该体系将大多数报道的Co/PMS体系中存在的HCO3-的负面影响转变为积极的影响，从而增强了AR1的脱色，使速率常数增加了2倍以上。增强的主要因素是高价钴氧中间体(PcCoIV=O)，它可能是通过CoPc-HCO3-络合物异源裂解PMS OO键而产生的。值得注意的是，作为主要活性物种的高价钴氧中间体不同于大多数已报道的Co/PMS体系的反应机理，在该体系中，羟基和硫酸根是主要的活性物种。本研究为开发高效的废水修复催化氧化技术奠定了基础。(C)2015爱思唯尔B.V.保留所有权利。
The design of catalytic oxidation processes with high efficiency has attracted considerable attention for a long while in environmental catalysis. In this work, a novel oxidation system, CFs-CoPc/PMS, was developed by coupling cellulosic fibers-bonded cobalt phthalocyanine (CFs-CoPc) with peroxymonosulfate (PMS). CFs-CoPc/PMS system could effectively decolorize azo dyes such as Acid Red 1 (AR1) with almost 100% decolorization efficiency in 35 min, suggesting that the CFs-CoPc/PMS system was a highly efficient oxidation process. In addition, bicarbonate ion (HCO3-) was further introduced to CFs-CoPc/PMS to construct a combined system, CFs-CoPc/PMS/HCO3-. Remarkably, this system turned the negative effect of HCO3- observed in most reported Co/PMS systems into a positive one, which enhanced the AR1 decolorization with over 2-fold increase of the rate constant. The main factor responsible for the enhancement was high-valent cobalt-oxo intermediates (PcCoIV=O), which was presumably generated via the heterolytic cleavage of the PMS OO bond by CoPc-HCO3- complex. It is noteworthy that high-valent cobalt-oxo intermediates as the major active species is different from most reported mechanisms in Co/PMS systems, in which hydroxyl and sulfate radicals are recognized as the dominant active species. This study paves an avenue for developing highly efficient catalytic oxidation technology for wastewater remediation. (C) 2015 Elsevier B.V. All rights reserved.