Ultrafast degradation of Cu(II)-EDTA by peroxymonosulfate activated with polyoxometalate clusters intercalated layered double hydroxides: Simultaneous decomplexation and resourcelization

IF 4.9 2区 化学 Q2 CHEMISTRY, PHYSICAL Colloids and Surfaces A: Physicochemical and Engineering Aspects Pub Date : 2024-11-26 DOI:10.1016/j.colsurfa.2024.135835
Jue Wang , Wenfang Shi , Wenqi Zhang , Hanxuan Zeng , Jing Deng , Haojie Zhang
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Abstract

Technologies used to handle metal pollution are often ineffective for complexed metals, which have refractory biodegradability, high solubility, and strong mobility, posing significant threats to the ecological environment. This work proposed a novel catalytic system for the proper disposal of Cu(II)-EDTA pollution. Polyoxometalate cluster intercalated CaFe layered double hydroxide (LDH-CoPW) prepared through a mild and convenience method was applied to activate peroxymonosulfate (PMS) for the degradation of Cu(II)-EDTA and the simultaneous immobilization of the released Cu(II). Compared to direct waste or complex regeneration of catalysts, the application of used LDH-CoPW in clean energy production was proposed to further reduce carbon emissions. Under the combination of 0.1 g/L of LDH CoPW and 0.1 mM of PMS, nearly 100 % of Cu(II)-EDTA was removed within 3 min of reaction time, and 49.6 % of Cu(II) was adsorbed within 60 min of reaction time. The second-order reaction kinetic constants of Co(IV) = O with various probes were confirmed by competition kinetics method. Based on this, Co(IV) = O was identified as the dominant RSs using a scientific probe-based kinetic model. Furthermore, CaFe-LDH did not directly activate PMS but ensured the reactivity of the catalytic system by promoting the redox cycle of cobalt species. Finally, due to the regulation of Cu on the electronic structure of the catalyst, the electrochemical performance of the used LDH-CoPW surpassed that of fresh LDH-CoPW and CaFe-LDH, showing great potential in clean energy production.
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过一硫酸盐在多氧金属簇插层双氢氧化物活化下对 Cu(II)-EDTA 的超快降解:同时解络合和资源化
络合金属具有难生物降解性、高溶解性和强流动性,对生态环境构成重大威胁,而用于处理金属污染的技术往往对络合金属无效。本研究提出了一种新型催化系统,用于妥善处理 Cu(II)-EDTA 污染。通过温和方便的方法制备的聚氧化金属簇插层 CaFe 层状双氢氧化物(LDH-CoPW)可活化过一硫酸盐(PMS),用于降解 Cu(II)-EDTA 并同时固定释放的 Cu(II)。与直接废弃或复合再生催化剂相比,建议将使用过的 LDH-CoPW 应用于清洁能源生产,以进一步减少碳排放。在 0.1 g/L LDH CoPW 和 0.1 mM PMS 的组合条件下,反应时间 3 分钟内,Cu(II)-EDTA 被去除近 100%,反应时间 60 分钟内,Cu(II)被吸附 49.6%。竞争动力学方法证实了 Co(IV) = O 与各种探针的二阶反应动力学常数。在此基础上,利用基于探针的科学动力学模型确定了 Co(IV) = O 为主要的 RSs。此外,CaFe-LDH 并不直接激活 PMS,而是通过促进钴物种的氧化还原循环来确保催化系统的反应活性。最后,由于 Cu 对催化剂电子结构的调节作用,使用过的 LDH-CoPW 的电化学性能超过了新鲜的 LDH-CoPW 和 CaFe-LDH,在清洁能源生产中显示出巨大的潜力。
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来源期刊
CiteScore
8.70
自引率
9.60%
发文量
2421
审稿时长
56 days
期刊介绍: Colloids and Surfaces A: Physicochemical and Engineering Aspects is an international journal devoted to the science underlying applications of colloids and interfacial phenomena. The journal aims at publishing high quality research papers featuring new materials or new insights into the role of colloid and interface science in (for example) food, energy, minerals processing, pharmaceuticals or the environment.
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