催化作用
纳米颗粒
化学
降级(电信)
热解
反应速率常数
胺气处理
化学工程
氮气
核化学
盐酸四环素
动力学
无机化学
四环素
有机化学
抗生素
工程类
物理
电信
量子力学
生物化学
计算机科学
作者
Qingqing Li,Jiadi Liu,Zhujuan Ren,Zikai Wang,Fei‐Fei Mao,Hua Wu,Rong Zhou,Yuanqing Bu
标识
DOI:10.1016/j.cej.2021.132269
摘要
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 m2 g−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 Co0 nanoparticles, Co-Nx/pyridinic N and graphitic N in C-Co-TN as catalytic active sites. The SO4·−, ·OH, O2·− and 1O2 were 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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