College of Environmental Science and Engineering, Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Changsha, 410082, P. R. China.
Small. 2020 Jul;16(29):e2001634. doi: 10.1002/smll.202001634. Epub 2020 Jun 22.
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 CoO bond and CoN 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.
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 CoO 键和 CoN 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。