College of Environment, Zhejiang University of Technology, Hangzhou 310014, China; School of Civil and Environmental Engineering, Nanyang Technological University (NTU), 50 Nanyang Avenue, Singapore 639798, Singapore.
Nanyang Environment and Water Research Institute (NEWRI), NTU, 1 Cleantech Loop, CleanTech One, Level 6, Singapore 637141, Singapore.
J Colloid Interface Sci. 2018 Jan 1;509:502-514. doi: 10.1016/j.jcis.2017.09.035. Epub 2017 Sep 8.
In this work, controllable preparation of micro/nanostructured bismuth ferrites (BFOs) were used to investigate multifarious heterogeneous catalyses, including Fenton/Fenton-like reaction, photocatalysis, photo-Fenton oxidation, and peroxymonosulfate (PMS) activation. Results showed that BFO can be used asa novel catalyst to activate switchable catalytic degradation of organic matters. Additionally, a novel catalytic system for degradation of organic pollutants, which integrating all-above heterogeneous catalyses is denoted as BFO/HO/PMS hybrid reaction, is introduced for the first time. BFO/HO/PMS system effectively degraded>99% for both methyl orange (MO) and sulfamethoxazole (SMX) within 60min, which shows better efficiency than above BFO-driven catalyses. The major SMX degradation pathway in BFO/HO/PMS system is proposed via detecting intermediates using LC/MS/MS. It was found that catalytic activities of BFOs are in the order of BFO-L (co-precipitation, micro/nanosize, single crystals exposing facet (001))>BFO-H (hydrothermal, nanocluster with a higher surface area than other BFOs)>BFO-C (fabricated using calcination process, microsize), which demonstrated that crystallographic orientation is more significant in heterogeneous catalyses than specific surface area at micro/nanoscale. Besides, the required HO consumption for achieving 99% TOC removal was identified in BFO-driven photo-Fenton oxidation. The other effects on degradation efficiency, such as HO dosage and pH, were investigated as well. In Fenton/Fenton-like reaction, reaction conditions suggested are ∼61.5mM HO dosage and pH≥4.5 to avoid quenching of HO into HO by excessive HO and Fe leaching.
在这项工作中,可控制备的微/纳米结构的铋铁氧体(BFOs)被用于研究各种多相催化反应,包括芬顿/Fenton 反应、光催化、光芬顿氧化和过一硫酸盐(PMS)活化。结果表明,BFO 可用作一种新型催化剂,以激活可切换的有机物质催化降解。此外,首次引入了一种新型的用于降解有机污染物的催化体系,该体系集成了上述所有多相催化反应,称为 BFO/HO/PMS 混合反应。BFO/HO/PMS 体系能在 60min 内有效降解>99%的甲基橙(MO)和磺胺甲恶唑(SMX),其效率明显优于上述 BFO 驱动的催化反应。通过使用 LC/MS/MS 检测中间体,提出了 BFO/HO/PMS 体系中 SMX 的主要降解途径。结果发现,BFOs 的催化活性顺序为 BFO-L(共沉淀,微/纳米尺寸,暴露(001)面的单晶)>BFO-H(水热,比其他 BFOs 具有更高表面积的纳米簇)>BFO-C(使用煅烧工艺制备,微尺寸),这表明在多相催化中晶面取向比微/纳米尺度的比表面积更重要。此外,在 BFO 驱动的光芬顿氧化中,确定了达到 99%TOC 去除所需的 HO 消耗。还研究了其他对降解效率的影响,如 HO 剂量和 pH 值。在芬顿/Fenton 反应中,建议的反应条件为~61.5mM 的 HO 剂量和 pH≥4.5,以避免过量 HO 和 Fe 浸出将 HO 猝灭为 HO。