High-loaded single Cu atoms decorated on N-doped graphene for boosting Fenton-like catalysis under neutral pH

被引:131
|
作者
Wu, Qianyuan [1 ]
Wang, Jin [2 ]
Wang, Zhiwei [3 ]
Xu, Yalan [3 ]
Xing, Zhihui [1 ]
Zhang, Xinyang [1 ]
Guan, Yuntao [1 ]
Liao, Guangfu [4 ]
Li, Xinzheng [1 ]
机构
[1] Tsinghua Univ, Tsinghua Shenzhen Int Grad Sch, Guangdong Prov Engn Res Ctr Urban Water Recycling, Key Lab Microorganism Applicat & Risk Control She, Shenzhen 518055, Peoples R China
[2] Shenzhen Univ, Coll Mat Sci & Engn, Shenzhen 518071, Peoples R China
[3] Tsinghua Berkeley Shenzhen Inst, China Shenzhen Environm Sci & New Energy Technol, Shenzhen 518055, Peoples R China
[4] Sun Yat Sen Univ, Guangdong Lab High Performance Polymer Composites, Minist Educ, Key Lab Polymer Composite & Funct Mat,Sch Mat Sci, Guangzhou 510275, Peoples R China
基金
中国国家自然科学基金;
关键词
OXYGEN REDUCTION; EFFICIENT ELECTROCATALYST; DEGRADATION; OXIDE; OXIDATION; CARBON; DECOLORIZATION; EVOLUTION; NITROGEN; EXCHANGE;
D O I
10.1039/d0ta04943c
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
Here, single-atom Cu dispersed on N-doped graphene (Cu-SA/NGO) with relatively high Cu loading of 5.8 wt% was prepared for boosting the degradation of contaminants. This is the highest value yet reported for dispersion of single metal atoms on graphene. Atomically dispersed CuN(4)moieties were confirmed by high-angle annular dark field-scanning transmission electron microscopy and X-ray absorption fine structure spectroscopy. The prepared Cu-SA/NGO shows remarkable activity and stability in the degradation of various organic contaminants at neutral pH. This excellent performance is mainly ascribed to the large number of active sites obtained from high single-atom-Cu loading. Density functional theory calculations confirmed that CuN(4)moieties serve as the active sites, with low energy barriers for hydroxyl radical ((OH)-O-center dot) generation. These supported single-atom catalysts (SACs) catalyze the heterogeneous Fenton reactionviaproton-mediated H2O2-homolytic pathway. This work offers a new method for fabricating various SACs with high loading levels for catalytic oxidation reactions.
引用
收藏
页码:13685 / 13693
页数:9
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