An efficient catalyst for carbamazepine degradation that alkali-etched silicon carbide Synergy effect with ZIF-67 (ZIF-67/AE-SiC) in peroxymonosulfate system

IF 13.3 1区 工程技术 Q1 ENGINEERING, CHEMICAL Chemical Engineering Journal Pub Date : 2025-01-18 DOI:10.1016/j.cej.2025.159685
Zhencong Liu, Zhiqi Zhu, Pengyuan Chen, Xiang Zhu, Fangdi Huang, Nannan Wang, Yan Qiu Zhu
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Abstract

Addressing the agglomeration issue of ZIF-67 is of great significance for its application in advanced oxidation processes (AOPs) targeting organic macromolecule pollutants. In this study, we etched commercially available silicon carbide (C-SiC) in an alkaline solution to obtain alkali-etched silicon carbide (AE-SiC). Using a co-precipitation method, we synthesized a composite material where ZIF-67 is surface-modified by AE-SiC (ZIF-67/AE-SiC). After alkali etching, AE-SiC particles become smaller, with increased porosity and larger pore size. These modifications allow AE-SiC to chemically bond to the surface of ZIF-67, effectively reducing its surface energy and thus resolving the issue of self-agglomeration. Meanwhile, the introduction of AE-SiC allows peroxymonosulfate (PMS) to enter ZIF-67 more rapidly, facilitating dynamic redox cycling in ZIF-67. This enhances the forming of reactive species like SO4·−, O2·−, and 1O2, leading to the production of additional free radicals that effectively degrade organic macromolecular pollutants. The optimized ZIF-67/AE-SiC(0.08) composite exhibited excellent catalytic activity in PMS-mediated carbamazepine (CBZ) degradation, achieving over 95% degradation within 8 min. A comprehensive investigation into the degradation pathways of CBZ was conducted, concurrently with an evaluation of the toxicity of itself and its degradation intermediates. This study expands the potential applications of silicon carbide and ZIF-67 materials in the development of PMS-based advanced oxidation processes.

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碱蚀碳化硅与ZIF-67 (ZIF-67/AE-SiC)在过氧单硫酸盐体系中协同作用的高效卡马西平降解催化剂
解决ZIF-67的团聚问题对其在有机大分子污染物的高级氧化工艺(AOPs)中的应用具有重要意义。在这项研究中,我们在碱性溶液中蚀刻市售碳化硅(C-SiC),得到碱蚀刻碳化硅(AE-SiC)。采用共沉淀法合成了以AE-SiC表面改性ZIF-67的复合材料(ZIF-67/AE-SiC)。碱蚀后,AE-SiC颗粒变小,孔隙率增大,孔径增大。这些修饰使得AE-SiC与ZIF-67表面化学键合,有效降低了ZIF-67的表面能,从而解决了自团聚问题。同时,AE-SiC的引入使过氧单硫酸盐(PMS)更快地进入ZIF-67,促进ZIF-67中的动态氧化还原循环。这增强了SO4·−、O2·−和1O2等活性物质的形成,导致产生额外的自由基,有效地降解有机大分子污染物。优化后的ZIF-67/AE-SiC(0.08)复合材料在pms介导的卡马西平(CBZ)降解中表现出优异的催化活性,在8 min内达到95%以上的降解效果。对CBZ的降解途径进行了全面的研究,同时对其本身及其降解中间体的毒性进行了评估。本研究拓展了碳化硅和ZIF-67材料在基于pms的高级氧化工艺开发中的潜在应用。
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来源期刊
Chemical Engineering Journal
Chemical Engineering Journal 工程技术-工程:化工
CiteScore
21.70
自引率
9.30%
发文量
6781
审稿时长
2.4 months
期刊介绍: The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.
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