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二氧化钛(P25)光催化修复二苯胂酸污染土壤:降解途径、操作参数优化及土壤性质的影响。

Diphenylarsinic acid contaminated soil remediation by titanium dioxide (P25) photocatalysis: Degradation pathway, optimization of operating parameters and effects of soil properties.

机构信息

Key Laboratory of Soil Environment and Pollution Remediation, Institute of Soil Science, Chinese Academy of Sciences, Nanjing 210008, China; Graduate School of Chinese Academy of Sciences, Beijing 100039, China.

Key Laboratory of Soil Environment and Pollution Remediation, Institute of Soil Science, Chinese Academy of Sciences, Nanjing 210008, China.

出版信息

Sci Total Environ. 2016 Jan 15;541:348-355. doi: 10.1016/j.scitotenv.2015.09.023. Epub 2015 Sep 25.

Abstract

Diphenylarsinic acid (DPAA) is formed during the leakage of arsenic chemical weapons in sites and poses a high risk to biota. However, remediation methods for DPAA contaminated soils are rare. Here, the photocatalytic oxidation (PCO) process by nano-sized titanium dioxide (TiO2) was applied to degrade DPAA in soil. The degradation pathway was firstly studied, and arsenate was identified as the final product. Then, an orthogonal array experimental design of L9(3)(4), only 9 experiments were needed, instead of 81 experiments in a conventional one-factor-at-a-time, was used to optimize the operational parameters soil:water ratio, TiO2 dosage, irradiation time and light intensity to increase DPAA removal efficiency. Soil:water ratio was found to have a more significant effect on DPAA removal efficiency than other properties. The optimum conditions to treat 4 g soil with a DPAA concentration of 20 mg kg(-1) were found to be a 1:10 soil: water ratio, 40 mW cm(-2) light intensity, 5% TiO2 in soil, and a 3-hour irradiation time, with a removal efficiency of up to 82.7%. Furthermore, this method (except for a change in irradiation time from 3 to 1.5h) was validated in nine different soils and the removal efficiencies ranged from 57.0 to 78.6%. Removal efficiencies were found to be negatively correlated with soil electrical conductivity, organic matter content, pH and total phosphorus content. Finally, coupled with electron spin resonance (ESR) measurement, these soil properties affected the generation of OH• by TiO2 in soil slurry. This study suggests that TiO2 photocatalytic oxidation is a promising treatment for removing DPAA from soil.

摘要

二苯胂酸(DPAA)是在场地砷化学武器泄漏过程中形成的,对生物群具有很高的风险。然而,DPAA 污染土壤的修复方法很少。在这里,纳米二氧化钛(TiO2)的光催化氧化(PCO)过程被应用于降解土壤中的 DPAA。首先研究了降解途径,鉴定出砷酸盐是最终产物。然后,采用 L9(3)(4)的正交数组实验设计,仅需 9 次实验,而不是传统的单因素逐一实验需要 81 次实验,优化了土壤比、TiO2 用量、辐照时间和光强等操作参数,以提高 DPAA 的去除效率。结果表明,土壤比相对于其他性质对 DPAA 去除效率的影响更大。处理 4g DPAA 浓度为 20mgkg(-1)的土壤的最佳条件为土壤:水比为 1:10、40mWcm(-2)的光强、土壤中 5%的 TiO2 和 3 小时的辐照时间,去除效率高达 82.7%。此外,该方法(除辐照时间从 3 小时改为 1.5 小时外)在 9 种不同的土壤中进行了验证,去除效率范围为 57.0%至 78.6%。去除效率与土壤电导率、有机质含量、pH 值和总磷含量呈负相关。最后,结合电子顺磁共振(ESR)测量,这些土壤性质影响了 TiO2 在土壤浆中的 OH•的生成。本研究表明,TiO2 光催化氧化是一种很有前途的处理 DPAA 污染土壤的方法。

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