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液滴流辅助多相电芬顿反应器降解β受体阻滞剂:响应面优化及机理阐明。

Droplet flow-assisted heterogeneous electro-Fenton reactor for degradation of beta-blockers: response surface optimization, and mechanism elucidation.

机构信息

Department of Chemistry, King Fahd University of Petroleum and Minerals, Dhahran, 31261, Saudi Arabia.

Department of Physics, KFUPM, Dhahran, 31261, Saudi Arabia.

出版信息

Environ Sci Pollut Res Int. 2019 May;26(14):14313-14327. doi: 10.1007/s11356-019-04551-1. Epub 2019 Mar 12.

Abstract

In this study, we report an effective degradation method for trace level beta-blockers (propranolol and acebutolol) in hospital wastewater using a new droplet flow-assisted heterogeneous electro-Fenton reactor (DFEF) system. Biogenic iron-carbon nanocomposites (RHS/C-x% Fe) as eco-friendly and low-cost heterogeneous Fenton catalysts were synthesized from rice husk via hydrolytic sol-gel routes. Here, we demonstrate the use of natural air as a nebulizing agent for fast and continuous catholyte air saturation and Fenton catalyst transfer to the cathode electrode. The effects of key operational parameters were evaluated and optimized using central composite design. Results clearly indicated that enhanced beta-blocker degradation was mainly dependent on the interactive effects of electrolysis time, current density, and catalyst dosage. Fast degradation efficiencies (≥ 99.9%) was recorded at neutral pH conditions. The decay followed pseudo-first-order kinetics with degradation rates of up to 2.72 × 10 and 2.54 × 10 min for acebutolol and propranolol, respectively. The synergistic contribution of OH attributable to DFEF process and OH for anodic oxidation (AO) at the anode electrode significantly enhanced the degradation process. Compared to AO, the conventional flow-assisted electro-Fenton (FEF), and the batch electro-Fenton (BEF), DFEF degradation efficiency followed a decreasing order: DFEF ˃ FEF ˃ BEF˃ AO. This trend in performance was mainly due to the fast and continuous cathodic electro-generation of HO and Fe regeneration. Additionally, in order to elucidate degradation mechanism, we used a combination of DFEF approach with liquid chromatography-tandem mass spectrometry analysis. This approach demonstrates a simple, cleaner, and highly efficient degradation approach for trace level recalcitrant pollutants in a complex aquatic matrix, without the need for external chemical addition and pH adjustment.

摘要

在这项研究中,我们报告了一种使用新型液滴流辅助非均相电芬顿反应器(DFEF)系统有效降解医院废水中痕量β-受体阻滞剂(普萘洛尔和醋丁洛尔)的方法。生物铁碳纳米复合材料(RHS/C-x% Fe)作为环保且低成本的非均相芬顿催化剂,是通过水解溶胶凝胶途径从稻壳中合成的。在这里,我们展示了使用自然空气作为雾化剂,以快速和连续地使阴极电解液饱和并将芬顿催化剂转移到阴极电极。使用中心复合设计评估和优化了关键操作参数的影响。结果清楚地表明,增强的β-受体阻滞剂降解主要取决于电解时间、电流密度和催化剂剂量的相互作用效应。在中性 pH 条件下,记录到快速降解效率(≥99.9%)。降解遵循准一级动力学,对于醋丁洛尔和普萘洛尔,降解速率分别高达 2.72×10 和 2.54×10 min。DFEF 过程中归因于 OH 的协同贡献和阳极电极处的阳极氧化(AO)的 OH 显著增强了降解过程。与 AO 相比,传统的流动辅助电芬顿(FEF)和分批电芬顿(BEF),DFEF 的降解效率遵循以下降序:DFEF ˃ FEF ˃ BEF˃ AO。这种性能趋势主要是由于快速和连续的阴极电化学产生 HO 和 Fe 再生。此外,为了阐明降解机制,我们使用 DFEF 方法与液相色谱-串联质谱分析相结合。该方法在无需外部化学添加和 pH 调节的情况下,展示了一种用于复杂水基质中痕量难降解污染物的简单、清洁和高效的降解方法。

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