Carbon Nitride Supported High-Loading Fe Single-Atom Catalyst for Activation of Peroxymonosulfate to Generate 1O2 with 100 % Selectivity
Dr. Long-Shuai Zhang
Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle, Nanchang Hangkong University, Nanchang, Jiangxi, 330063 P. R. China
These authors contributed equally to this work.
Search for more papers by this authorDr. Xun-Heng Jiang
Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle, Nanchang Hangkong University, Nanchang, Jiangxi, 330063 P. R. China
These authors contributed equally to this work.
Search for more papers by this authorZi-Ai Zhong
Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle, Nanchang Hangkong University, Nanchang, Jiangxi, 330063 P. R. China
Search for more papers by this authorLei Tian
Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle, Nanchang Hangkong University, Nanchang, Jiangxi, 330063 P. R. China
Search for more papers by this authorQing Sun
Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle, Nanchang Hangkong University, Nanchang, Jiangxi, 330063 P. R. China
Search for more papers by this authorProf. Yi-Tao Cui
SANKA High Technology Co. Ltd. 90-1, Kurimachi, Shingu-machi, Tatsuno, Hyogo, 679-5155 Japan
Search for more papers by this authorProf. Xin Lu
State Key Laboratory of Physical Chemistry of Solid Surface, Xiamen University, Xiamen, Fujian, 361005 P. R. China
Search for more papers by this authorCorresponding Author
Prof. Jian-Ping Zou
Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle, Nanchang Hangkong University, Nanchang, Jiangxi, 330063 P. R. China
Search for more papers by this authorProf. Sheng-Lian Luo
Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle, Nanchang Hangkong University, Nanchang, Jiangxi, 330063 P. R. China
Search for more papers by this authorDr. Long-Shuai Zhang
Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle, Nanchang Hangkong University, Nanchang, Jiangxi, 330063 P. R. China
These authors contributed equally to this work.
Search for more papers by this authorDr. Xun-Heng Jiang
Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle, Nanchang Hangkong University, Nanchang, Jiangxi, 330063 P. R. China
These authors contributed equally to this work.
Search for more papers by this authorZi-Ai Zhong
Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle, Nanchang Hangkong University, Nanchang, Jiangxi, 330063 P. R. China
Search for more papers by this authorLei Tian
Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle, Nanchang Hangkong University, Nanchang, Jiangxi, 330063 P. R. China
Search for more papers by this authorQing Sun
Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle, Nanchang Hangkong University, Nanchang, Jiangxi, 330063 P. R. China
Search for more papers by this authorProf. Yi-Tao Cui
SANKA High Technology Co. Ltd. 90-1, Kurimachi, Shingu-machi, Tatsuno, Hyogo, 679-5155 Japan
Search for more papers by this authorProf. Xin Lu
State Key Laboratory of Physical Chemistry of Solid Surface, Xiamen University, Xiamen, Fujian, 361005 P. R. China
Search for more papers by this authorCorresponding Author
Prof. Jian-Ping Zou
Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle, Nanchang Hangkong University, Nanchang, Jiangxi, 330063 P. R. China
Search for more papers by this authorProf. Sheng-Lian Luo
Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle, Nanchang Hangkong University, Nanchang, Jiangxi, 330063 P. R. China
Search for more papers by this authorGraphical Abstract
The carbon nitride supported Fe single-atom catalyst (Fe1/CN) with a Fe loading of 11.2 wt % was developed to generate 100 % 1O2 by activating peroxymonosulfate (PMS). The adsorption of terminal O and oxidation of PMS by Fe-N4 sites played the most important roles for 1O2 generation with 100 % selectivity. As a result, the Fe1/CN activated PMS system exhibited strong resistance to various factors during the degradation of organic pollutants.
Abstract
Singlet oxygen (1O2) is an excellent active species for the selective degradation of organic pollutions. However, it is difficult to achieve high efficiency and selectivity for the generation of 1O2. In this work, we develop a graphitic carbon nitride supported Fe single-atoms catalyst (Fe1/CN) containing highly uniform Fe-N4 active sites with a high Fe loading of 11.2 wt %. The Fe1/CN achieves generation of 100 % 1O2 by activating peroxymonosulfate (PMS), which shows an ultrahigh p-chlorophenol degradation efficiency. Density functional theory calculations results demonstrate that in contrast to Co and Ni single-atom sites, the Fe-N4 sites in Fe1/CN adsorb the terminal O of PMS, which can facilitate the oxidization of PMS to form SO5.−, and thereafter efficiently generate 1O2 with 100 % selectivity. In addition, the Fe1/CN exhibits strong resistance to inorganic ions, natural organic matter, and pH value during the degradation of organic pollutants in the presence of PMS. This work develops a novel catalyst for the 100 % selective production of 1O2 for highly selective and efficient degradation of pollutants.
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