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利用太阳能激活过氧化钙衰减油砂处理水中与苯并萘酸有关的物质:实验因素的影响、机理建模和毒性评估。

Attenuation of phenylnaphthenic acids related to oil sands process water using solar activated calcium peroxide: Influence of experimental factors, mechanistic modeling, and toxicity evaluation.

机构信息

Department of Civil and Environmental Engineering, University of Alberta, T6G 1H9, Edmonton, AB, Canada; Key Laboratory of Organic Compound Pollution Control Engineering (MOE), School of Environmental and Chemical Engineering, Shanghai University, Shanghai 200444, PR China.

Department of Civil and Environmental Engineering, University of Alberta, T6G 1H9, Edmonton, AB, Canada.

出版信息

Water Res. 2024 Oct 1;263:122188. doi: 10.1016/j.watres.2024.122188. Epub 2024 Jul 30.

Abstract

Refractory naphthenic acids (NAs) are among the primary toxic compounds in oil sands process water (OSPW), a matrix with a complex chemical composition that poses challenges to its remediation. This study evaluated the effectiveness of calcium peroxide (CaO) combined with solar radiation (solar/CaO) as an advanced water treatment process for degrading model NAs (1,2,3,4-tetrahydronaphthalene-2-carboxylic acid, pentanoic acid, and diphenylacetic acid) in synthetic water (STW) and provide preliminary insights in treating real OSPW. Solar light and CaO acted synergistically to degrade target NAs in STW (>67 of synergistic factor) following a pseudo-first-order kinetic (R ≥ 0.95), with an optimal CaO dosage of 0.1 g L. Inorganic ions and dissolved organic matter were found to hinder the degradation of NAs by solar/CaO treatment; however, the complete degradation of NAs was reached in 6.7 h of treatment. The main degradation mechanism involved the generation of hydroxyl radicals (OH), which contributed ∼90% to the apparent degradation rate constant (K), followed by HO (4-5%) and O (0-5%). The tentative transformation pathways of three NAs were proposed, confirming an open-ring reaction and resulting in short-chain fatty acid ions as final products. Furthermore, a reduction in acute microbial toxicity and genotoxic effect was observed in the treated samples, suggesting that solar/CaO treatment exhibits high environmental compatibility. Furthermore, the solar/CaO system was successfully applied as a preliminary step for real-world applications to remove natural NAs, fluorophore organic compounds, and inorganic components from OSPW, demonstrating the potential use of this technology in the advanced treatment of oil-tailing-derived NAs.

摘要

难处理的环烷酸(NAs)是油砂开采废水(OSPW)中的主要毒性化合物之一,该基质具有复杂的化学成分,这对其修复构成了挑战。本研究评估了过碳酸钠(CaO)与太阳辐射(solar/CaO)联合作为一种先进的水处理工艺,用于降解合成水中(STW)的模型 NAs(1,2,3,4-四氢萘-2-羧酸、戊酸和二苯乙酸),并初步探讨了处理实际 OSPW 的可能性。太阳光照和 CaO 协同作用,在 STW 中对目标 NAs 进行降解(协同因子>67),遵循准一级动力学(R≥0.95),最佳 CaO 剂量为 0.1 g/L。研究发现,无机离子和溶解的有机物会阻碍 solar/CaO 处理对 NAs 的降解;然而,在 6.7 小时的处理后,NAs 完全降解。主要的降解机制涉及羟基自由基(OH)的生成,这对表观降解速率常数(K)的贡献约为 90%,其次是 HO(4-5%)和 O(0-5%)。提出了三种 NAs 的可能转化途径,证实了开环反应,最终产物为短链脂肪酸离子。此外,处理后的样品中观察到急性微生物毒性和遗传毒性效应降低,表明 solar/CaO 处理具有较高的环境相容性。此外,该 solar/CaO 系统成功地应用于实际应用的初步步骤,从 OSPW 中去除天然 NAs、荧光有机化合物和无机成分,表明该技术在油砂衍生 NAs 的深度处理方面具有应用潜力。

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