Integration of Atomically Dispersed Cu–N4 Sites with C3N4 for Enhanced Photo-Fenton Degradation over a Nonradical Mechanism
Integration of Atomically Dispersed Cu–N4 Sites with C3N4 for Enhanced Photo-Fenton Degradation over a Nonradical Mechanism
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原子分散的 Cu-N4 位点与 C3N4 的整合，通过非自由基机制增强光芬顿降解
DOI：
10.1021/acsestengg.2c00261
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发表时间：
2022
期刊：
影响因子：
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通讯作者：
Zhiyi Lu
中科院分区：
文献类型：
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作者：
Shuqian Dong;Xu Chen;Linfeng Su;Yingjie Wen;Yuechu Wang;Qihao Yang;Li Yi;Wenwen Xu;Qiu Yang;Peilei He;Yunqing Zhu;Zhiyi Lu
Photo-Fenton降解法作为一种很有前途的抗生素废水处理方法受到了广泛关注，但其催化性能不理想严重限制了其工业应用。在此，我们证明，限制原子分散的Cu到C3 N4（Cu-C3 N4），使快速H2 O2活化和光生电子-空穴对的有效分离，导致在一个显着的改善的光芬顿反应的降解效率。优化的Cu-C3 N4催化剂对环丙沙星（CIP）的光Fenton降解率在30 min内接近99%，其准一级反应速率常数为0.0978 min-1，是纯C3 N4催化剂的4.5倍。电子顺磁共振、猝灭实验和X射线吸收精细结构分析结果表明，该上级Photo-Fenton催化剂的催化性能是由O·Cu-N4·O中间体的形成激活H2 O2的非自由基反应途径所决定的.这种新型催化剂以及新颖的H2 O2活化机理对废水处理领域的材料设计具有重要意义。
Photo-Fenton degradation as a promising strategy for antibiotic wastewater treatment attracted extensive attention, while the unsatisfactory catalytic performance vitally limits its industrial application. Herein, we demonstrate that confining atomically dispersed Cu into C3N4(Cu–C3N4) enables fast H2O2activation and efficient separation of photogenerated electron–hole pairs, resulting in a dramatic improvement of the degradation efficiency of the Photo-Fenton reaction. Photo-Fenton degradation of ciprofloxacin (CIP) was close to 99% within 30 min over optimized Cu–C3N4, corresponding to a pseudo-first-order rate constant of ∼0.0978 min–1, almost 4.5 times higher than pure C3N4counterpart. The electron paramagnetic resonance, quenching experiments, and X-ray absorption fine structure results reveal that the superior Photo-Fenton catalytic performance is attributed to a nonradical reaction pathway, where the H2O2is activated by the formation of the O═Cu–N4═O intermediate. The advanced catalyst as well as the refreshing H2O2activation mechanism are of profound significance for the materials design in the wastewater treatment field.