Degradation of Typical Nitrogen-Heterocyclic Compounds in Coal Gasification Wastewater via Catalytic Ozonation Processes

IF 4.3 3区 材料科学 Q1 ENGINEERING, ELECTRICAL & ELECTRONIC ACS Applied Electronic Materials Pub Date : 2024-11-07 DOI:10.1007/s11270-024-07516-4
Pengkang Zhang, Bangguo Liu, Tao Zhao, Jiayu Yu, Xiaoyun Ye, Xiurong Chen
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Abstract

Reverse osmosis is a critical step in the pursuit of zero discharge for coal gasification wastewater treatment; however, the high-salt concentrates generated in this process contain refractory organic compounds, such as indole, quinoline, and pyridine, which pose significant challenges for salt recovery. In this study, catalytic ozonation using a novel Cu-Co-Mn/activated carbon catalyst was introduced to efficiently degrade these persistent organic pollutants. The optimized conditions were a pH of 9.0, a catalyst dosage of 1.3 g/L, and an ozone dosage of 1.0 g/L. Our findings reveal that the catalytic effect promotes the accumulation of hydroxyl-free radicals, which provide the necessary energy for effective degradation. The removal efficiencies of indole, quinoline, and pyridine by catalytic ozonation were remarkably high at 92.31%, 90.56%, and 80.63%, respectively. Pyridine, identified as the most resistant compound, had its electronic structure calculated using density functional theory (DFT) with Gaussian 09 software, offering new insights into the underlying degradation processes. The results demonstrate that the novel catalyst significantly boosts ozonation efficiency, offering a promising approach for treating high-salt coal gasification wastewater.

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通过催化臭氧工艺降解煤气化废水中的典型氮杂环化合物
反渗透是实现煤气化废水处理零排放的关键步骤;然而,该工艺中产生的高盐浓缩物含有难降解的有机化合物,如吲哚、喹啉和吡啶,这给盐回收带来了巨大挑战。本研究采用新型铜-钴-锰/活性炭催化剂进行催化臭氧氧化,以有效降解这些持久性有机污染物。优化条件为 pH 值为 9.0、催化剂用量为 1.3 克/升、臭氧用量为 1.0 克/升。我们的研究结果表明,催化作用促进了无羟自由基的积累,而无羟自由基为有效降解提供了必要的能量。臭氧催化法对吲哚、喹啉和吡啶的去除率非常高,分别为 92.31%、90.56% 和 80.63%。吡啶是抗性最强的化合物,利用高斯 09 软件通过密度泛函理论(DFT)对其电子结构进行了计算,为了解其降解过程提供了新的视角。研究结果表明,新型催化剂能显著提高臭氧氧化效率,为处理高盐煤气化废水提供了一种前景广阔的方法。
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CiteScore
7.20
自引率
4.30%
发文量
567
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