高效可见光响应 ZnFe₂O₄/MXene 的制备及光催化性能

Preparation and Photocatalytic Performance of Highly Efficient Visible-light Responsive ZnFe₂O₄/MXene

摘要

ZnFe₂O₄作为光催化剂易被可见光激发、环境毒性低且磁性易回收，在有机废水处理中具有良好的应用前景. 然而，ZnFe₂O₄的光生电子-空穴对易复合限制了其光催化活性. 本文结合水热法和室温静电吸附法制备了ZnFe₂O₄/MXene光催化剂，并通过自身形貌调控(微米棒、中空微球、阿基米德多面体、“爆米花”球、纳米颗粒)和MXene的协同作用解决了ZnFe₂O₄可见光下光催化效率不佳的问题. 借助MXene的高导电性，光催化剂的电荷转移效率得到改善，光生载流子易分离. 当ZnFe₂O₄呈阿基米德多面体，MXene用量为ZnFe₂O₄的10%时，ZnFe₂O₄/MXene对亚甲基蓝(MB)的降解率在20 min内可达到96.9%，分别为ZnFe₂O₄和MXene的2.1和3.0倍；循环5次后，MB降解率仍保持在90.0%以上. 通过X射线光电子能谱价带谱和活性物种捕获实验提出了ZnFe₂O₄/MXene对MB的降解机理，起主要作用的活性物种为^∙O₂⁻，^∙OH和h⁺起次要作用.

Abstract

ZnFe₂O₄, a visible-light-responsive photocatalyst, exhibits significant potential for organic wastewater treatment due to its low environmental toxicity and magnetic recyclability. However, the rapid recombination of photogenerated electron-hole pairs in pure ZnFe₂O₄ severely limits its photocatalytic activity. To address this issue, ZnFe₂O₄/MXene photocatalysts were developed via a combined hydrothermal and room-temperature electrostatic adsorption approach. Additionally, the photocatalytic efficiency of ZnFe₂O₄ under visible light was enhanced through the morphology control of ZnFe₂O₄(microrod, hollow microsphere, Archimedean polyhedron, “popcorn” sphere, nanoparticle) and the synergistic effect of MXene. The high conductivity of MXene improved charge transfer efficiency and facilitated the separation of photogenerated carriers. When ZnFe₂O₄ was synthesized as an Archimedean polyhedron and MXene dosage was 10% of ZnFe₂O₄, the optimized ZnFe₂O₄/MXene photocatalyst achieved a methylene blue(MB) degradation efficiency of 96.9% within 20 min, which was 2.1 and 3.0 times higher than that of ZnFe₂O₄ and MXene, respectively. Moreover, the degradation efficiency of MB remained over 90.0% after five cycles. The degradation mechanism of MB by ZnFe₂O₄/MXene was investigated using valence band spectrum of X-ray photoelectron spectroscopy and active species capture experiments. The results indicated that ^∙O₂ ⁻ served as the primary active species, while ^∙OH and h⁺ played secondary roles in MB degradation.

关键词

可见光光催化剂 / ZnFe₂O₄ / MXene / 亚甲基蓝 / 磁性

Key words

Visible-light photocatalyst / ZnFe₂O₄ / MXene / Methylene blue / Magnetic

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基金资助

国家自然科学基金(22278256)

陕西省创新能力支撑计划项目(2025ZC-KJXX-41)