Insights into adsorption and high photocatalytic oxidation of ciprofloxacin under visible light by intra-molecular Donor-Acceptor like p-n isotype heterojunction: Performance and mechanism
Insights into adsorption and high photocatalytic oxidation of ciprofloxacin under visible light by intra-molecular Donor-Acceptor like p-n isotype heterojunction: Performance and mechanism
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DOI：
10.1016/j.cej.2023.142533
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发表时间：
2023-03
影响因子：
15.1
通讯作者：
Mingjuan Zhang;Yi Zhang;Yuan Zhu;Jiajia Wang;Lu Qiao;Yue Zhao;Yani Tao;Yao-Yu Xiao;Lin Tang
中科院分区：
文献类型：
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作者：
Mingjuan Zhang;Yi Zhang;Yuan Zhu;Jiajia Wang;Lu Qiao;Yue Zhao;Yani Tao;Yao-Yu Xiao;Lin Tang
天然水和污水中经常检测到环丙沙星(CIP)等抗生素，然而，由于抑制了细菌的增殖，传统的污水处理技术对有效去除这些抗生素提出了巨大的挑战。本文合成了磷、硼共掺空心管状g-C_3N_4(xB-PCN)类分子内给体型同质异质结，用于高效可见光催化降解CIP。Mott-Schottky曲线表明，xB-PCN同时具有p型和n型电导，这可能是因为掺杂的硼具有电子受体效应，NH/NH_2基团可以作为电子给体。这种独特的性质使xB-PCN具有良好的电荷产生、分离和转移能力，能够高效地光降解CIP，1h内分解效率达到87.56%，表观速率常数(0.01151−1)是PCN的6.85倍。此外，3B-PCN在自来水(84.63%)和养殖废水(78.41%)中保持了较高的降解率。LC-MS和TOC分析结果表明，CIP逐渐矿化，并提出了降解途径。基于自由基捕集实验和ESR表征，验证了CIP降解过程中所涉及的活性氧物种。这项工作为基于无金属共轭聚合物g-C3N4的抗生素污染水的处理提供了一条很有前途的途径。
Antibiotics, e.g. ciprofloxacin (CIP) are frequently detected in natural waters and sewage, however, the conventional sewage treatment techniques presents a great challenge for efficient removal them due to the inhibition of bacterial proliferation. Herein, the intra-molecular Donor-Acceptor like p-n isotype heterojunction of phosphorus and boron co-doped hollow tubular g-C3N4(xB-PCN) was synthesized for high-efficiency visible light photocatalytic degradation of CIP. The Mott-Schottky curves showed that the xB-PCN exhibited both p and n-type conductivities, which probably because the doped boron has electron acceptor effect and the NH/NH2groups could act as electron donors. This unique property enables xB-PCN to have excellent charge generation, separation and transfer ability for the highly efficient photodegradation of CIP, reaching 87.56% of decomposition efficiency within 1 h with the apparent rate constant (0.01151 min−1) of 6.85 times that of PCN. Furthermore, the 3B-PCN maintained high degradation percentage in tap water (84.63%) and aquaculture wastewater (78.41%). The results of LC-MS and TOC showed that CIP was gradually mineralized and the degradation pathways were proposed. Based on the radical trapping experiments and ESR characterization, the reactive oxygen species involved in the degradation of CIP were checked. This work offers a promising approach for treating antibiotics polluted water based on a metal-free conjugated polymeric g-C3N4.