Catalytic degradation of antibiotic by Co nanoparticles encapsulated in nitrogen-doped nanocarbon derived from Co-MOF for promoted peroxymonosulfate activation

Catalytic degradation of antibiotic by Co nanoparticles encapsulated in nitrogen-doped nanocarbon derived from Co-MOF for promoted peroxymonosulfate activation
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封装在 Co-MOF 衍生的氮掺杂纳米碳中的 Co 纳米颗粒催化降解抗生素,促进过一硫酸盐活化

DOI:
10.1016/j.cej.2021.132269
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发表时间:
2022
影响因子:
15.1
通讯作者:
Yuanqing Bu
Yuanqing Bu
中科院分区:
工程技术1区
文献类型:
--
作者:
Qingqing Li;Jiadi Liu;Zhujuan Ren;Zikai Wang;Feifei Mao;Hua Wu;Rong Zhou;Yuanqing Bu

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同时,合理优化和设计催化剂的结构和组成是进一步提高催化剂性能的重要途径。在本论文中,我们成功地制备了一种新型磁性材料(C-Co-TN),将Co纳米颗粒包裹在掺氮纳米碳中,作为过一硫酸盐(PMS)活化催化剂。首次以Co-TN(Co(TTPA)(4-NBA)(H2O)2]·4-NBA·0.5DMF,TTPA=三(1-(1H-1,2,4-三唑-1-基)苯基)胺)为前驱体,通过一步热解将Co-TN中的Co离子和N-配体分别转化为Co纳米粒子和掺氮碳层,得到了衍生物C-Co-TN。C-Co-TN具有较大的比表面积(258.40 m2g−1),在30min内对盐酸四环素(TCH)的降解活性比纯Co-TN高93.3%,其中C-Co-TN/PMS体系对TCH的降解动力学常数是Co-TN/PMS体系的3倍。在较宽的pH值范围内,TCH的最终降解率保持在94%以上,TOC的最终降解率可达47%。较高的TCH去除效率归因于纳米CoO、C-Co-TN中的Co-NX/吡啶N和石墨化N作为催化活性中心。在C-Co-TN/PMS体系中,SO4·−、·OH、O2·−和10O2共存。这项工作不仅为将MOF转化为具有优异催化性能的磁性催化剂用于水修复提供了可能,而且也为研究掺氮多孔炭诱导多相催化的非自由基途径提供了基础。
Simultaneously rational optimization and design of the structure and composition are extremely significant approaches to further improve the performances of catalysts. Herein, a novel magnetic material (C-Co-TN) of Co nanoparticles encapsulated in nitrogen-doped nanocarbon was successfully fabricated as a peroxymonosulfate (PMS) activation catalyst. The derivative C-Co-TN was obtained from one new MOFs of Co-TN (Co(TTPA)(4-Nba)(H2O)2]·4-Nba·0.5DMF, TTPA = tris(4-(1H-1,2,4-triazol-1-yl)phenyl)amine) as a precursor for the first time, in which the Co ions and N-ligands of Co-TN were respectively transformed to Co nanoparticles and nitrogen-doped carbon layer via a one-step pyrolysis. The C-Co-TN with a large specific surface area (258.40 m2g−1) displayed excellent PMS activation for tetracycline hydrochloride (TCH) degradation with 93.3% efficiency within 30 min superior to the pure Co-TN, in which the obtained kinetic constant for TCH removal in the C-Co-TN/PMS system was 3 times greater than Co-TN/PMS system. The final degradation rate of TCH was maintained above 94% in a wide pH range of 4–9, and 47% of TOC could be eliminated. The higher TCH removal efficiency was attributed to Co0nanoparticles, Co-Nx/pyridinic N and graphitic N in C-Co-TN as catalytic active sites. The SO4·−,·OH, O2·−and1O2were coexisted in C-Co-TN/PMS system. The work not only provides a possibility for converting MOFs into magnetic catalyst with excellent catalytic performance for water remediation, but also gives underlying insight in non-free radical pathways of heterogeneous catalysis induced by nitrogen-doped porous carbon.
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发表时间: 2021-03-24
影响因子: 10.9
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发表时间: 2019-05
期刊: Applied Catalysis B: Environmental
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影响因子: 15.1
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