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二硫代苏糖醇(Dithionite)在厌氧条件下去除四溴双酚 A 的优化及机制:响应面法和降解途径。

Optimization and mechanism of Tetrabromobisphenol A removal by dithionite under anaerobic conditions: Response surface methodology and degradation pathway.

机构信息

School of Civil and Environmental Engineering, Harbin Institute of Technology (Shenzhen), Shenzhen, 518055, China.

School of Civil and Transportation Engineering, Guangdong University of Technology, Guangzhou, 510006, China.

出版信息

J Environ Manage. 2022 Nov 1;321:116034. doi: 10.1016/j.jenvman.2022.116034. Epub 2022 Aug 23.

Abstract

In this study, dithionite (DTN) was used to degrade Tetrabromobisphenol A (TBBPA), a widely applied brominated flame retardants, under anaerobic conditions with the reaction terminator of nitrate. The optimization of reaction parameters including TBBPA concentration, DTN concentration and pH value were conducted by response surface methodology (RSM) based on central composite design (CCD). The degradation process could be simulated accurately by a quadratic model with the correlation coefficient R of 0.9550. The interaction between pH and DTN concentration was significant with the p-value of 0.0017. Moreover, the maximum TBBPA removal was 87.6 ± 3.2% and obtained at TBBPA concentration of 2.00 μM, the DTN concentration of 322.31 μM, and the pH of 6.14 under anaerobic conditions. It was found that the factors influenced TBBPA removal followed the order: pH > DTN concentration > TBBPA concentration. The major active products from DTN are SO and SO. In addition, different inhibitions of natural water matrix including chloride, bicarbonate, sulfide and humic acid on TBBPA degradation had been confirmed. According to the identified six intermediates via gas chromatography-mass spectrometry (GC-MS), two steps of the degradation pathways were speculated, including the breakage of C-Br bond and C-C bond. This study provides a convenient way to degrade TBBPA.

摘要

在这项研究中,使用连二亚硫酸钠(DTN)在硝酸盐的反应终止剂存在下,在厌氧条件下降解四溴双酚 A(TBBPA),一种广泛应用的溴化阻燃剂。通过基于中心复合设计(CCD)的响应面法(RSM)对包括 TBBPA 浓度、DTN 浓度和 pH 值在内的反应参数进行了优化。降解过程可以通过二次模型准确模拟,相关系数 R 为 0.9550。pH 值和 DTN 浓度之间的相互作用具有显著意义,p 值为 0.0017。此外,在厌氧条件下,当 TBBPA 浓度为 2.00 μM、DTN 浓度为 322.31 μM、pH 值为 6.14 时,TBBPA 的最大去除率为 87.6±3.2%。结果表明,影响 TBBPA 去除的因素顺序为:pH 值>DTN 浓度>TBBPA 浓度。DTN 的主要活性产物为 SO 和 SO。此外,还确认了包括氯化物、碳酸氢盐、硫化物和腐殖酸在内的天然水基质对 TBBPA 降解的不同抑制作用。通过气相色谱-质谱联用仪(GC-MS)鉴定出的六种中间产物表明,降解途径包括 C-Br 键和 C-C 键的断裂。本研究为降解 TBBPA 提供了一种便捷的方法。

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