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通过 ZVZ 固定化 g-CN 实现高效强化臭氧化性能,以实现对微量污染物的优越氧化。

Efficient enhancement of ozonation performance via ZVZ immobilized g-CN towards superior oxidation of micropollutants.

机构信息

School of Environmental Engineering, Wuhan Textile University, Wuhan 430073, China; Engineering Research Center for Clean Production of Textile Dyeing and Printing, Ministry of Education, Wuhan 430073, China.

School of Environmental Engineering, Wuhan Textile University, Wuhan 430073, China.

出版信息

Chemosphere. 2018 Aug;205:369-379. doi: 10.1016/j.chemosphere.2018.04.121. Epub 2018 Apr 21.

Abstract

A functional organic-metal composite material zero-valent zinc immobilized graphitic carbon nitride (ZVZ-g-CN) was prepared by a fast and facile two-step synthetic approach with an optimal ZVZ content of 5.4 wt%. The structure, surface morphology and chemical composition of the as-synthesized ZVZ-g-CN were characterized by BET surface area, XRD, FT-IR, SEM, TEM, and XPS, respectively. ZVZ-g-CN composite exhibited superior catalytic ozonation activity with an improvement of 61.2% on atrazine (ATZ) degradation efficiency in 1.5 min reaction, more than 12 times of the pseudo-first-order rate constant, and almost 16-fold of the R value obtained in O/ZVZ-g-CN process compared to O alone. Meanwhile, the ATZ degradation efficiency was gradually enhanced with increasing ZVZ-g-CN dosage and initial solution pH in the range from 3.0 to 9.0, and a higher amount of ATZ was degraded when the initial concentration of ATZ rose from 1 to 10 mg L. The enhanced catalytic ozonation activity of ZVZ-g-CN is attributed to the synergistic effects among ZVZ, ZnO and g-CN, as well as the improved dispersibility, increased surface area, and intensive electron-transfer ascribed to the electronic and surface properties modification. The radical scavengers experiments demonstrated that O, OH, and O were the dominant reactive radical species in the multifunctional processes. Moreover, an empirical kinetic model was proposed to predict ATZ degradation. The results indicated that the ZVZ-g-CN composite was a highly efficient, recoverable, and durable catalyst, which would provide a promising alternative in catalytic ozonation.

摘要

一种功能化有机金属复合材料零价锌固载石墨相氮化碳(ZVZ-g-CN),采用快速简便的两步合成法制备,最佳 ZVZ 含量为 5.4wt%。采用 BET 比表面积、XRD、FT-IR、SEM、TEM 和 XPS 分别对合成的 ZVZ-g-CN 的结构、表面形貌和化学成分进行了表征。ZVZ-g-CN 复合材料表现出优异的催化臭氧化活性,在 1.5 min 的反应中,阿特拉津(ATZ)的降解效率提高了 61.2%,比单独的 O 获得的表观一级速率常数提高了 12 倍以上,R 值提高了近 16 倍。同时,随着 ZVZ-g-CN 用量和初始溶液 pH 值从 3.0 增加到 9.0,ATZ 的降解效率逐渐提高,当 ATZ 的初始浓度从 1 mg·L 增加到 10 mg·L 时,降解的 ATZ 量更高。ZVZ-g-CN 增强的催化臭氧化活性归因于 ZVZ、ZnO 和 g-CN 之间的协同作用,以及电子和表面性质改性引起的分散性提高、表面积增加和电子转移增强。自由基捕获实验表明,O、OH 和 O 是多相过程中的主要活性自由基。此外,提出了一个经验动力学模型来预测 ATZ 的降解。结果表明,ZVZ-g-CN 复合材料是一种高效、可回收和耐用的催化剂,在催化臭氧化中具有广阔的应用前景。

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