ZIF-8 assisted synthesis of magnetic core-shell Fe3O4@CuS nanoparticles for efficient sulfadiazine degradation via H2O2 activation: Performance and mechanism.
ZIF-8 assisted synthesis of magnetic core-shell Fe3O4@CuS nanoparticles for efficient sulfadiazine degradation via H2O2 activation: Performance and mechanism.
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DOI：
10.1016/j.jcis.2021.03.057
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发表时间：
2021-03
影响因子：
9.9
通讯作者：
Haojie Zhang;Chan Zhou;Hanxuan Zeng;Huiying Wu;Ling-fang Yang;Lin Deng;Zhou Shi
中科院分区：
文献类型：
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作者：
Haojie Zhang;Chan Zhou;Hanxuan Zeng;Huiying Wu;Ling-fang Yang;Lin Deng;Zhou Shi
以咪唑骨架分子筛（ZIF）为模板剂，采用化学刻蚀和阳离子交换法合成了新型磁性核壳结构Fe3O4@CuS。形貌和微结构表征表明，Fe3O4@CuS纳米粒子为菱形十二面体结构，稳定性高，具有磁性，比表面积大（772.20 m2/g）。通过H2 O2活化法评估了Fe 3 O4@CuS对磺胺嘧啶（SDZ）降解的催化活性。充分考察了影响SDZ去除的多种因素。用0.2 g/L Fe3O4@CuS和5 mM H2 O2在90 min内去除约93.2% SDZ（50 μM）。特别地，Fe3O4@CuS在3.0-11.0的宽pH范围内表现出优质的催化性能。自由基清除实验和电子顺磁共振（EPR）分析证实，·O2-、·OH和1 O2均对SDZ的降解有贡献，其中·OH起主导作用。机理研究表明，Fe3O4@CuS的有效催化活性主要是由于CuS壳层上的硫增强铜基芬顿反应、Fe 3 O 4核层上的硫增强铁基芬顿反应以及壳核之间的有效电子传递。最后，在中间体鉴定的基础上，进一步提出了SDZ可能的降解途径。本工作提出了一种以ZIF-8为模板合成磁性核壳结构Fe3O4@CuS的新策略，该模板具有优异的H2 O2活化降解SDZ的性能。
A novel magnetic core–shell Fe3O4@CuS have been successfully synthesized by chemical etching and cation exchange method using Zeolitic imidazolate frameworks (ZIF) as the template. The morphology and microstructural properties characterization indicated that Fe3O4@CuS nanoparticles were rhombic dodecahedral shape, highly stable, and magnetic with a large specific surface area (772.20 m2/g). The catalytic activity of Fe3O4@CuS was assessed on sulfadiazine (SDZ) degradation by H2O2activation. Multi-factors affecting the SDZ removal was adequately investigated. Approximately 93.2% SDZ (50 μM) was removed with 0.2 g/L Fe3O4@CuS and 5 mM H2O2in 90 min. In particular, Fe3O4@CuS exhibited a quality catalytic performance within a wide pH range of 3.0–11.0. Radical scavenger tests and electron paramagnetic resonance (EPR) analysis confirmed that •O2−, •OH, and1O2all contributed to the SDZ degradation, and •OH played the dominant role. Meanwhile, mechanism investigation suggested that the effective catalytic activity of Fe3O4@CuS could be ascribed to the sulphur-enhanced copper-based Fenton reaction on the CuS shell, sulphur-enhanced iron-based Fenton reaction on the Fe3O4core, and the effective electron transfer between the shell and core. Finally, the possible SDZ degradation pathways were further proposed on the basis of the intermediates identification. This work put forward a new strategy to synthesize magnetic core–shell Fe3O4@CuS using ZIF-8 as the template with outstanding performance for H2O2activation to degrade SDZ.