Hierarchical nano-vesicles with bimetal-encapsulated for peroxymonosulfate activation: singlet oxygen-dominated oxidation process
Hierarchical nano-vesicles with bimetal-encapsulated for peroxymonosulfate activation: singlet oxygen-dominated oxidation process
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用于过一硫酸盐活化的双金属封装的分层纳米囊泡：单线态氧主导的氧化过程
DOI：
10.1016/j.cej.2021.133581
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发表时间：
2021-11
影响因子：
15.1
通讯作者：
Philippe François-Xavier Corvini
中科院分区：
文献类型：
--
作者：
Zhiping Lyu;Menglu Xu;Jinnan Wang;Aimin Li;Philippe François-Xavier Corvini
设计了双层纳米囊泡（FeCu1.5O3@NV），用于过一硫酸盐（PMS）的1O2主导氧化活化。与以往的核壳型催化剂不同，FeCu1. 5O3被包裹在空心沸石球中，这些沸石球单元组装成分级纳米囊泡。FeCu1.5O3@NV具有介孔结构和丰富的内腔，可使反应物富集于内腔，增强与活性中心的接触。氧化物的柔性表面增强了与表面吸附物和底物的亲和力，加速了反应物之间的电子转移。密度泛函理论计算表明，FeCu1.5O3@NV对BPA和PMS具有较强的结合能力，促进了PMS的活化和BPA在空心球单元内的降解.由于氧化还原电对和纳米囊泡结构的协同作用，BPA降解过程中可通过两条途径产生大量的1O2.第一条途径是氧化还原电对与PMS之间的反应，第二条途径是O2·−的链式反应。由于FeCu1.5O3@NV均匀地封装在分级纳米囊泡中，因此具有高的催化稳定性，金属浸出可忽略不计。即使在5次循环后，BPA去除率仍然可以保持100%。
Hierarchical nano-vesicles with bimetal-encapsulated (FeCu1.5O3@NV) was designed for peroxymonosulfate (PMS) activation with the1O2-dominated oxidation process. Different from previous core–shell metal-loaded catalysts, FeCu1.5O3was encapsulated in hollow zeolite spheres, and these zeolite sphere units assembled to construct hierarchical nano-vesicles. Owning to mesoporous shell and abundant interior cavity, FeCu1.5O3@NV could enrich reactants in cavity for enhancing the contact with active sites. The flexible surface of bimetal oxides strengthened the affinity with surface adsorbates and substrates, accelerating the electron transfer between reactants. DFT calculation indicated that FeCu1.5O3@NV possessed strong binding affinity for BPA and PMS, facilitating PMS activation and BPA degradation inside of hollow sphere units. Being attributed to the synergistic effect of bimetal redox couples and hierarchical nano-vesicle structure, large amounts of1O2could be generated through two pathways for BPA degradation. The first pathway is the reaction between bimetal redox couples and PMS, and the second is the chain reaction of O2•−. Due to bimetal oxides uniformly encapsulated in hierarchical nano-vesicles, FeCu1.5O3@NV possessed high catalytic stability with negligible metal leaching. Even after 5 cycles, BPA removal could still remain 100%.
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期刊：
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