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金属掺杂碳负载/修饰钛酸盐纳米管用于水中全氟辛烷磺酸盐的降解:制备条件、机制的影响及参数优化。

Metal-doped carbon-supported/modified titanate nanotubes for perfluorooctane sulfonate degradation in water: Effects of preparation conditions, mechanisms, and parameter optimization.

机构信息

Environmental Engineering Program, Department of Civil and Environmental Engineering, Auburn University, Auburn, AL 36849, USA.

School of Resource and Geosciences, China University of Mining and Technology, Xuzhou, Jiangsu 221116, China.

出版信息

Sci Total Environ. 2022 Dec 20;853:158573. doi: 10.1016/j.scitotenv.2022.158573. Epub 2022 Sep 6.

Abstract

Metal-doped, activated carbon (AC) supported titanate nanotubes (Me/TNTs@AC) have been shown promising for photocatalytic degradation of per- and polyfluoroalkyl substances (PFAS). However, the preparation recipe of the adsorptive photocatalysts has not yet been optimized in terms of type and content of precursor ACs and the metal dopants as well as synthesizing conditions. In this work, the photocatalytic performance of Me/TNTs@AC was evaluated based on the effectiveness in defluorination of pre-sorbed perfluorooctane sulfonic acid (PFOS) after 4-h UV irradiation. Based on the experimental results, the highest photocatalytic mineralization efficiency (66.2 %) of PFOS was achieved using Ga/TNTs@AC prepared under the following conditions: Filtrosorb-400® = 50 wt%, Ga = 2 wt%, hydrothermal treatment temperature = 130 °C, hydrothermal duration = 72 h, and calcination temperature = 550 °C. To understand the underlying mechanisms, selected materials were characterized via X-ray diffraction, the BET surface area and pore volume, UV-vis diffuse reflectance spectrometry, and photoluminescence. The results revealed that the superior photoactivity of Ga/TNTs@AC is attributed to the Ga-facilitated formation of pure crystallized anatase phase during the calcination, high UV light absorption, formation of microscale hybrid AC-anatase-Ga phases, and oxygen defects induced by Ga. The information can facilitate preparation and optimization of composite photocatalysts for efficient adsorption and photocatalytic degradation of PFAS in water.

摘要

金属掺杂的、负载在钛酸盐纳米管上的活性炭(Me/TNTs@AC)在光催化降解全氟和多氟烷基物质(PFAS)方面表现出了很好的前景。然而,在吸附光催化剂的制备方案中,前驱体活性炭的类型和含量、金属掺杂剂以及合成条件等方面还没有得到优化。在这项工作中,基于 4 小时紫外光照后预吸附的全氟辛烷磺酸(PFOS)的脱氟效果,评估了 Me/TNTs@AC 的光催化性能。根据实验结果,使用在以下条件下制备的 Ga/TNTs@AC 实现了最高的 PFOS 光催化矿化效率(66.2%):Filtrosorb-400®=50wt%、Ga=2wt%、水热处理温度=130°C、水热时间=72h、煅烧温度=550°C。为了理解潜在的机制,通过 X 射线衍射、BET 比表面积和孔体积、紫外-可见漫反射光谱和光致发光对所选材料进行了表征。结果表明,Ga/TNTs@AC 的优越光活性归因于 Ga 促进煅烧过程中形成纯结晶锐钛矿相、高紫外光吸收、形成微尺度混合 AC-锐钛矿-Ga 相以及 Ga 诱导的氧缺陷。这些信息有助于制备和优化用于水中高效吸附和光催化降解 PFAS 的复合光催化剂。

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