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在具有双齿配体的聚合碳氮化物上原位生长的单原子钴用于高效光催化降解难处理抗生素。

In Situ Grown Single-Atom Cobalt on Polymeric Carbon Nitride with Bidentate Ligand for Efficient Photocatalytic Degradation of Refractory Antibiotics.

机构信息

College of Environmental Science and Engineering, Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Changsha, 410082, P. R. China.

出版信息

Small. 2020 Jul;16(29):e2001634. doi: 10.1002/smll.202001634. Epub 2020 Jun 22.

DOI:10.1002/smll.202001634
PMID:32567191
Abstract

Semiconductor photocatalysis is a promising technology to tackle refractory antibiotics contamination in water. Herein, a facile in situ growth strategy is developed to implant single-atom cobalt in polymeric carbon nitride (pCN) via the bidentate ligand for efficient photocatalytic degradation of oxytetracycline (OTC). The atomic characterizations indicate that single-atom cobalt is successfully anchored on pCN by covalently forming the CoO bond and CoN bond, which will strengthen the interaction between single-atom cobalt and pCN. This single-atom cobalt can efficiently expand optical absorption, increase electron density, facilitate charge separation and transfer, and promote OTC degradation. As the optimal sample, Co(1.28%)pCN presents an outstanding apparent rate constant for OTC degradation (0.038 min ) under visible light irradiation, which is about 3.7 times than that of the pristine pCN. The electron spin resonance (ESR) tests and reactive species trapping experiments demonstrate that the O , h , •O , and •OH are responsible for OTC degradation. This work develops a new way to construct single-atom-modified pCN and provides a green and highly efficient strategy for refractory antibiotics removal.

摘要

半导体光催化是一种很有前途的技术,可以解决水中难降解抗生素的污染问题。在此,通过双齿配体发展了一种简便的原位生长策略,将单原子钴植入聚合物氮化碳(pCN)中,用于高效光催化降解土霉素(OTC)。原子特征表明,单原子钴通过与 pCN 形成 CoO 键和 CoN 键成功地锚定在 pCN 上,这将增强单原子钴与 pCN 之间的相互作用。这种单原子钴可以有效地扩展光吸收,增加电子密度,促进电荷分离和转移,并促进 OTC 的降解。作为最佳样品,Co(1.28%)pCN 在可见光照射下对 OTC 的降解表现出出色的表观速率常数(0.038 min ),约为原始 pCN 的 3.7 倍。电子自旋共振(ESR)测试和活性物种捕获实验表明, O 、 h 、 •O 、和 •OH 是 OTC 降解的原因。这项工作开发了一种构建单原子修饰 pCN 的新方法,为去除难降解抗生素提供了一种绿色高效的策略。

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