Peroxydisulfate activation by photo-generated charges on mesoporous carbon nitride for removal of chlorophenols
Peroxydisulfate activation by photo-generated charges on mesoporous carbon nitride for removal of chlorophenols
复制标题
介孔氮化碳上光生电荷活化过二硫酸盐去除氯酚
DOI：
10.1016/j.apcatb.2021.120370
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发表时间：
2021
期刊：
影响因子：
--
通讯作者：
Qian Xufang
中科院分区：
文献类型：
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作者：
Liu Guimin;Zhang Ting;Wang Tian;Yamashita Hiromi;Zhao Yixin;Qian Xufang
在可见光照射下，光生电荷参与过硫酸氢盐（PDS）在介孔氮化碳（MCN）上的路易斯碱基活化。光生空穴（h+）、超氧自由基（O2·−）和单线态氧（1O2）是去除2,4,6-三氯苯酚（TCP）最重要的活性物质。MCN的Lewis碱基位点诱导PDS界面水解生成氢过氧阴离子（HOO−）和过氧化物离子（O22−），并与h+反应生成O2·−和2o。有效分离的电子（e−）负责对TCP的c单键cl键的亲核攻击。此外，vis/MCN/PDS的每阶电能（EEO）（3.75 × 106kW h m−3order−1）比UV/PDS的每阶电能（3.14 × 107kW h m−3order−1）低一个数量级。本文重点介绍了具有Lewis碱基的无金属MCN作为光催化剂活化PDS，并阐明了PDS活化去除氯酚污染物的新策略。
Photogenerated charges were found to involve in activation of peroxydisulfate (PDS) on mesoporous carbon nitride (MCN) with Lewis basic sites under visible light irradiation. Photogenerated hole (h+), superoxide radical (O2·−) and singlet oxygen (1O2) were verified as the most important active species for 2,4,6-trichlorophenol (TCP) removal. Lewis basic sites of MCN induced the interface hydrolysis of PDS to produce hydroperoxyl anions (HOO−) and peroxide ions (O22−), which was further reacted with h+to generate O2·−and1O2predominantly. The efficiently separated electron (e−) was responsible for the nucleophilic attack toward the Csingle bondCl bond of TCP. Moreover, the electrical energy per order (EEO) of vis/MCN/PDS (3.75 × 106kW h m−3order−1) was an order of magnitude lower than that of UV/PDS (3.14 × 107kW h m−3order−1). This work highlighted the metal-free MCN with Lewis basic sites as a photocatalyst to activate PDS and elucidated a new strategy of PDS activation for chlorophenol pollutants removal.