Bimetallic CoMn-MOF decorated biochar as peroxymonosulfate activator for efficient ofloxacin degradation: Performance and mechanism insights

IF 7.2 2区 工程技术 Q1 ENGINEERING, CHEMICAL
Long Zhang , Minghan Cao , Junying Song , Mengxiang Hui
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Abstract

The application of metal-organic framework (MOF)-based peroxymonosulfate (PMS) catalysts in heterogeneous reactions has attracted widespread interests. However, improving the efficiency and stability of the catalysts remains considerable challenges. Herein, bimetallic CoMn-MOF was constructed on the surface of biochar derived from peanut shell to fabricate the CoMn-MOF/biochar (CMB) composite as PMS catalyst using a simple hydrothermal process. Under optimal degradation conditions, i.e., [CMB] = 1 g/L, [PMS] = 1 mM, the ofloxacin (OFL) degradation efficiency can reach 92.9 % in 120 min in CMB/PMS system, and in which the reaction rate constant (0.1075 min−1) was 82 times higher than that in CoMn-MOF/PMS (0.0013 min−1). The remarkable improved catalytic performance was attributed to the multi active sites CMB composite enhanced electron transfer rate to produce abundant reaction active species. Besides, CMB exhibited high OFL degradation efficiency (77.8 %) after five cycles and strong mineralization efficiency (66.2 %) by effectively activating PMS. Moreover, the toxicity of OFL and its intermediates after degradation was greatly reduced based on the TEST results. The primary active species identified in this study were O2•-, 1O2 and SO4•- for OFL degradation in the CMB/PMS system. Furthermore, based on the results of the quenching experiments and HPLC-MS analysis, a catalytic degradation mechanism for OFL was proposed along with three potential degradation pathways. This research proposes a novel reference to develop an effective PMS catalyst for wastewater treatment through the combination of biochar and bimetallic MOFs.
双金属共聚物修饰的生物炭作为氧氟沙星高效降解的过氧单硫酸盐活化剂:性能和机制的见解
基于金属有机骨架(MOF)的过氧单硫酸根(PMS)催化剂在非均相反应中的应用引起了广泛的关注。然而,提高催化剂的效率和稳定性仍然是一个相当大的挑战。本文在花生壳生物炭表面构建双金属common - mof,采用简单的水热法制备common - mof /生物炭(CMB)复合材料作为PMS催化剂。在[CMB] = 1 g/L, [PMS] = 1 mM的最佳降解条件下,CMB/PMS体系在120 min内对氧氟沙星(OFL)的降解效率可达92.9 %,反应速率常数(0.1075 min−1)是con - mof /PMS体系(0.0013 min−1)的82倍。多活性位点CMB复合材料提高了电子传递速率,产生了丰富的反应活性物质,从而显著提高了催化性能。此外,经过5次循环后,CMB表现出较高的OFL降解效率(77.8% %)和较强的矿化效率(66.2% %)。此外,根据测试结果,降解后的OFL及其中间体的毒性大大降低。在CMB/PMS系统中,降解OFL的主要活性物质为O2•-、1O2和SO4•-。此外,基于淬灭实验和HPLC-MS分析结果,提出了OFL的催化降解机理以及三种可能的降解途径。本研究为生物炭与双金属mof的结合开发有效的PMS废水处理催化剂提供了新的参考。
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来源期刊
Journal of Environmental Chemical Engineering
Journal of Environmental Chemical Engineering Environmental Science-Pollution
CiteScore
11.40
自引率
6.50%
发文量
2017
审稿时长
27 days
期刊介绍: The Journal of Environmental Chemical Engineering (JECE) serves as a platform for the dissemination of original and innovative research focusing on the advancement of environmentally-friendly, sustainable technologies. JECE emphasizes the transition towards a carbon-neutral circular economy and a self-sufficient bio-based economy. Topics covered include soil, water, wastewater, and air decontamination; pollution monitoring, prevention, and control; advanced analytics, sensors, impact and risk assessment methodologies in environmental chemical engineering; resource recovery (water, nutrients, materials, energy); industrial ecology; valorization of waste streams; waste management (including e-waste); climate-water-energy-food nexus; novel materials for environmental, chemical, and energy applications; sustainability and environmental safety; water digitalization, water data science, and machine learning; process integration and intensification; recent developments in green chemistry for synthesis, catalysis, and energy; and original research on contaminants of emerging concern, persistent chemicals, and priority substances, including microplastics, nanoplastics, nanomaterials, micropollutants, antimicrobial resistance genes, and emerging pathogens (viruses, bacteria, parasites) of environmental significance.
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