Zhang Liang, Zhang Bofan, Wang Li, Ge Rile, Zhou Wenhui, Kubuki Shiro, Wu Ren'an, Wang Junhu
Center for Advanced Mössbauer Spectroscopy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China; University of Chinese Academy of Sciences, Beijing 100049, China.
Department of Chemistry, Tokyo Metropolitan University, Tokyo 192-0397, Japan.
J Colloid Interface Sci. 2022 Feb 15;608(Pt 3):3098-3110. doi: 10.1016/j.jcis.2021.11.042. Epub 2021 Nov 13.
A novel heterogeneous catalyst PB@MoS was successfully synthesized via facile hydrothermal processes and identified as a superior peroxymonosulfate (PMS) activator for organic pollutants degradation under visible light irradiation. The MoS nanosheet is uniformly adhered to the surface of iron-based metal-organic framework Prussian blue (PB) cube, exhibiting a tightly hydrangeas-like structure. Benefiting from strongly interfacial interaction (FeMo-sulfide) between PB and MoS, as confirmed by Fe M̈össbauer spectra and electrochemical measurement, the PB@MoS catalyst significantly accelerate the charge carrier transfer via interfacial FeMo-sulfide and thereby improve PMS activation ability to generate abundant reactive radicals. Moreover, the crucial iron active site was steadily validated by introduction of sodium oxalate trapping agent and visible light. In summary, the visible light induced Fenton-like reaction over PB@MoS catalyst promoted the Fe/Fe cycling and electron transport and further triggered the reactive species (SO, OH, O and h) productivity, realizing an extraordinarily high degradation and mineralization efficiency for various refractory organic pollutants. This work would provide a deep insight into develop heterogeneous Fe-based metal organic framework/MoS catalyst for environmental restoration and remediation by photo-Fenton reaction.
通过简便的水热法成功合成了一种新型的多相催化剂PB@MoS,并确定其为可见光照射下用于降解有机污染物的优异过一硫酸盐(PMS)活化剂。MoS纳米片均匀地附着在铁基金属有机框架普鲁士蓝(PB)立方体表面,呈现出紧密的绣球花状结构。通过Fe穆斯堡尔光谱和电化学测量证实,得益于PB和MoS之间强烈的界面相互作用(FeMo-硫化物),PB@MoS催化剂通过界面FeMo-硫化物显著加速电荷载流子转移,从而提高PMS活化能力以产生大量活性自由基。此外,通过引入草酸钠捕获剂和可见光,关键的铁活性位点得到了稳定验证。总之,PB@MoS催化剂上可见光诱导的类芬顿反应促进了Fe/Fe循环和电子传输,并进一步触发了活性物种(SO、OH、O和h)的产生,实现了对各种难降解有机污染物极高的降解和矿化效率。这项工作将为开发用于环境修复和光芬顿反应的多相铁基金属有机框架/MoS催化剂提供深入见解。