污染物
催化作用
光催化
双金属片
苯酚
电子顺磁共振
降级(电信)
化学
碳纤维
羟基化
化学工程
可重用性
光化学
材料科学
有机化学
工程类
物理
复合材料
复合数
酶
电信
程序设计语言
核磁共振
软件
计算机科学
作者
Xin Li,Zhiyu Yang,Guosheng Wu,Yizhe Huang,Zhikeng Zheng,Hector F. Garcés,Kai Yan
标识
DOI:10.1016/j.cej.2022.136066
摘要
• The NCC (NiCo 2 O 4 grown on carbon) is developed as a robust photo-Fenton-like catalyst. • The synergistic effect between NC and carbon enhances the catalytic performance. • The NCC + PMS + L coupling system is universal for phenolic pollutants removal. • Degradation intermediates and removal mechanisms are identified and elucidated. Rational design of photocatalysts with the controllable structure to expose active sites is crucial to degrade phenolic pollutants. Herein, we report the in-situ synthesis of lily-like NiCo 2 O 4 nanosheets (0.95 nm) grown on waste biomass-derived carbon (abbreviated as NCC) for the highly efficient photocatalytic removal of phenolic pollutants through the integration of experiment and theory calculation. These as-fabricated NCC photocatalysts (2.29 nm) exhibit superior performance for the fast removal of phenolic pollutants (such as 4-Acetamidophenol (AP), phenol, and aspirin) in comparison with their counterpart and previously reported candidates. By using AP as a model molecule for mimicking pollutants, the photocatalytic degradation performance of NCC nanosheets is ∼ 1.3 and 1.9 times higher than that of pure NiCo 2 O 4 (NC) and porous carbon, respectively. Various factors that influenced the degradation process such as peroxymonosulfate (PMS) concentration, catalyst dosage, AP concentration, and initial pH are thoroughly investigated. The free radical quenching experiments and electron paramagnetic resonance (EPR) spectra further demonstrate the existence of SO 4 − ·, ·OH, ·O 2 – , and 1 O 2 in the reaction system and the ·O 2 – radical play a major role, which is also confirmed by the density functional theory (DFT) calculation. Several degradation pathways (e.g., demethylation, deacylation, hydroxylation, and ring-opening) are then proposed based on the detected intermediates. Finally, the high stability and good reusability of NCC nanosheets are confirmed via the degradation efficiency of over 85% even after five successive cycles.
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