期刊
CHEMICAL ENGINEERING JOURNAL
卷 446, 期 -, 页码 -出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.136759
关键词
CoS@FeS; Heterostructure; Sulfur vacancies; Peroxymonosulfate; Sulfamethoxazole
资金
- National Natural Science Foundation of China [52100001, 51978032]
- Joint project of Beijing Municipal Education Commission and Municipal Nature Science Foundation [21JH0024]
- Youth Beijing Scholars program, China [024]
The incorporation of heterostructure and vacancies in the CoS@FeS catalyst synergistically triggers peroxymonosulfate (PMS) activation, leading to the efficient degradation of sulfamethoxazole (SMX) through a non-radical/radical oxidized pathway. Sulfur vacancies (SVs) facilitate the adsorption of PMS and dissolved oxygen (DO) on the catalyst surface, while the heterostructure enhances the charge transfer efficiency. The integration of SVs with heterostructure reduces the adsorption energy of PMS on the catalyst interface and improves the charge transfer efficiency for PMS activation.
The incorporation of heterostructure and vacancies will bring new strategies to improve the intrinsic activity of catalysts. Herein, the CoS@FeS heterostructure catalyst with sulfur vacancies (SVs) was fabricated by a simple hydrothermal strategy, which can synergistically trigger peroxymonosulfate (PMS) activation toward the efficient degradation of sulfamethoxazole (SMX) (k(obs), 0.3334 min(-1)) through a non-radical/radical oxidized pathway. SO4 center dot-, center dot OH and O-1(2) were regarded as the main reactive oxygen species (ROSs). Mechanism studies revealed that the synergy of SVs and heterostructure played an electron density adjusting role for the PMS activation into SO4 center dot- and center dot OH, as well as the continuous generation of center dot O-2 from O-2, thereby in favor of O-1(2). The SVs availed the adsorption of PMS and dissolved oxygen (DO) on the surface, the continuous electron transmission would be consolidated through the charge transfer efficiency (CTE) of heterostructure. Meanwhile, the integration of SVs with heterostructure reduced the adsorption energy of PMS (-3.82 eV) on the interface of the catalyst according to the density functional theory (DFT) calculations, which overcame the repulsion effect between negatively charged HSO5- and CoS@FeS, and enhanced the charge transfer efficiency to accelerate the PMS activation for generating SO4 center dot- and center dot OH. This work will propose a new approach for synergistically stimulating the intrinsic activity of catalysts to improve environmental remediation.
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