Nitrogen-doped carbon-coated Cu 0 activates molecular oxygen for norfloxacin degradation over a wide pH range

被引:6
作者
Liu, Yanjing [1 ]
Wang, Ruitao [2 ]
Liu, Shuhong [1 ]
Xu, Yunsong [1 ]
Zhang, Zhirong [3 ]
Song, Ying [1 ]
Yao, Zhongping [1 ]
机构
[1] Harbin Inst Technol, Sch Chem & Chem Engn, State Key Lab Urban Water Resource & Environm, Harbin 150001, Peoples R China
[2] Tianjin Univ, Ningbo Key Lab Green Petrochem Carbon Emiss Reduct, Zhejiang Inst, Ningbo 315201, Peoples R China
[3] Yancheng Inst Technol, Sch Chem & Chem Engn, Yancheng 224051, Peoples R China
基金
中国国家自然科学基金;
关键词
Fenton-like; Molecular oxygen activation; Metal-organic framework; Cu0/NC; Antibiotic degradation; ZERO-VALENT COPPER; OXIDATIVE-DEGRADATION; FACILE PREPARATION; WASTE-WATER; NANOPARTICLES; REDUCTION; MECHANISM; ACID; IRON; ACETAMINOPHEN;
D O I
10.1016/j.jcis.2024.03.189
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The Fenton -like activated molecular oxygen technology demonstrates significant potential in the treatment of refractory organic pollutants in wastewater, offering promising development prospects. We prepared a N -doped C -coated copper -based catalyst Cu 0 /NC3-600 through the pyrolysis of Mel -modified Cu -based metal - organic framework (MOF). The results indicate that the degradation of 20 mg/L norfloxacin (NOR) was achieved using 1.0 g/L Cu 0 /NC3-600 across a wide pH range, with a removal rate exceeding 95 % and total organic carbon (TOC) removals approaching 70 % after 60 min at pH 5 - 11. The nitrogen doping enhances the electronic structure of the carbon material, facilitating the adsorption of molecular oxygen. Additionally, the formed carbon layer effectively prevent copper leaching,contributing to increased stability to a certain extent. Subsequently, we propose the catalytic reaction mechanism for the Cu 0 /NC/air system. Under acidic conditions, Cu 0 /NC3-600 activates molecular oxygen to produce the center dot O 2 - , which serves as the primary active species for NOR degradation. While in alkaline conditions, the high-valent copper species Cu 3 + is generated in conjunction with center dot O 2 - , both working simultaneously for NOR degradation. Furthermore, based on the LC -MS results, we deduced four possible degradation pathways. This work offers a novel perspective on expanding the pH range of copper -based catalysts with excellent ability to activate molecular oxygen for environmental water treatment.
引用
收藏
页码:945 / 957
页数:13
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