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