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一种新型生物炭负载赤泥催化剂的制备及应用:活性位与催化机理。

Preparation and application of a novel biochar-supported red mud catalyst:Active sites and catalytic mechanism.

机构信息

Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, Kunming 650500, China; Guangdong Provincial Engineering Research Center for Online Monitoring of Water Pollution, Guangdong Provincial Key Laboratory of Emergency Test for Dangerous Chemicals, Guangdong Institute of Analysis (China National Analytical Center Guangzhou), Guangdong Academy of Sciences, Guangzhou 510000, China.

Guangdong Provincial Engineering Research Center for Online Monitoring of Water Pollution, Guangdong Provincial Key Laboratory of Emergency Test for Dangerous Chemicals, Guangdong Institute of Analysis (China National Analytical Center Guangzhou), Guangdong Academy of Sciences, Guangzhou 510000, China; College of Petrochemical Engineering, Lanzhou University of Technology, Lanzhou 730000, China.

出版信息

J Hazard Mater. 2021 Apr 15;408:124802. doi: 10.1016/j.jhazmat.2020.124802. Epub 2020 Dec 9.

Abstract

A novel catalyst RM-BC was synthesized by hydrothermal treatment and pyrolysis (800 ℃) using red mud and coconut shells. Influence of different preparation conditions on catalyst performance was explored. SEM showed that RM-BC was porous and RM was successfully loaded on the outside surface and inside the pores of BC. XRD revealed that FeO in RM was reduced to Fe and FeO in the pyrolysis process, in which pyrolysis temperature and addition ratio of coconut shells were critical. TGA-MS, FT-IR and XPS were also applied to character the catalyst. 100% of AO7 was removed within 30 min with conditions of 2 mM PS, 50 mg/L AO7 and 0.5 g/L RM-BC, and the Fe leaching was negligible. High removal rate was obtained in tap, river, and lake water. RM-BC/PS system also exhibited excellent degradation performance for other dyes (MB, MG and RhB) and antibiotics (TC, OTC and CTC). The mechanism studies demonstrated that PS was mainly activated by Fe and Fe in RM-BC to produce different radicals, then O was generated by the reactions among these radicals to degrade AO7. Finally, nine intermediate products of AO7 were identified by FT-ICR-MS and a probable degradation pathway was proposed.

摘要

采用水热法和热解法(800℃),以赤泥和椰子壳为原料合成了一种新型催化剂 RM-BC。考察了不同制备条件对催化剂性能的影响。SEM 表明,RM-BC 具有多孔性,RM 成功负载在 BC 的外表面和孔内。XRD 表明,RM 中的 FeO 在水热过程中被还原为 Fe,在热解过程中进一步被还原为 FeO,其中热解温度和椰子壳添加量是关键因素。TGA-MS、FT-IR 和 XPS 也被用于表征催化剂。在 PS 浓度为 2 mM、AO7 浓度为 50 mg/L、RM-BC 用量为 0.5 g/L 的条件下,AO7 可在 30 min 内被完全去除,且 Fe 的浸出可忽略不计。在自来水、河水和湖水等多种水体中均能获得较高的去除率。RM-BC/PS 体系对其他染料(MB、MG 和 RhB)和抗生素(TC、OTC 和 CTC)也表现出优异的降解性能。机理研究表明,PS 主要通过 RM-BC 中的 Fe 和 Fe 活化产生不同的自由基,然后通过这些自由基之间的反应生成 O 来降解 AO7。最后,通过 FT-ICR-MS 鉴定了 AO7 的 9 个中间产物,并提出了可能的降解途径。

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