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通过光敏剂与钒酸铋之间的客体-主体协同作用实现抗生素的高效光降解:潜在机制与毒性评估

Effective photodegradation of antibiotics by guest-host synergy between photosensitizer and bismuth vanadate: Underlying mechanism and toxicity assessment.

作者信息

Tan Meihong, Shi Wanping, Wang Haifeng, Di Guanglan, Xie Zhengxin, Fan Shisuo, Tang Jun, Dong Fengshou

机构信息

School of Resource and Environment, Anhui Agricultural University, Hefei, 230036, China.

School of Resource and Environment, Anhui Agricultural University, Hefei, 230036, China.

出版信息

Chemosphere. 2023 Jun;325:138362. doi: 10.1016/j.chemosphere.2023.138362. Epub 2023 Mar 9.

DOI:10.1016/j.chemosphere.2023.138362
PMID:36905996
Abstract

The removal of antibiotics in wastewater has attracted increasing attention. Herein, a superior photosensitized photocatalytic system was developed with acetophenone (ACP) as the guest photosensitizer, bismuth vanadate (BiVO) as the host catalyst and poly dimethyl diallyl ammonium chloride (PDDA) as the bridging complex, and used for the removal of sulfamerazine (SMR), sulfadiazine (SDZ) and sulfamethazine (SMZ) in water under simulated visible light (λ > 420 nm). The obtained ACP-PDDA-BiVO nanoplates attained a removal efficiency of 88.9%-98.2% for SMR, SDZ and SMZ after 60 min reaction and achieved kinetic rate constant approximately 10, 4.7 and 13 times of BiVO, PDDA-BiVO and ACP-BiVO, respectively, for SMZ degradation. In the guest-host photocatalytic system, ACP photosensitizer was found to have a great superiority in enhancing the light absorption, promoting the surface charge separation-transfer and efficient generation of holes (h) and superoxide radical (·O), greatly contributing to the photoactivity. The SMZ degradation pathways were proposed based on the identified degradation intermediates, involving three main pathways of rearrangement, desulfonation and oxidation. The toxicity of intermediates was evaluated and the results demonstrated that the overall toxicity was reduced compared with parent SMZ. This catalyst maintained 92% photocatalytic oxidation performance after five cyclic experiments and displayed a co-photodegradation ability to others antibiotics (e.g., roxithromycin, ciprofloxacin et al.) in effluent water. Therefore, this work provides a facile photosensitized strategy for developing guest-host photocatalysts, which enabling the simultaneous antibiotics removal and effectively reduce the ecological risks in wastewater.

摘要

废水中抗生素的去除已引起越来越多的关注。在此,开发了一种优异的光敏光催化体系,以苯乙酮(ACP)作为客体光敏剂,钒酸铋(BiVO)作为主体催化剂,聚二甲基二烯丙基氯化铵(PDDA)作为桥连配合物,并用于在模拟可见光(λ > 420 nm)下去除水中的磺胺甲嘧啶(SMR)、磺胺嘧啶(SDZ)和磺胺二甲嘧啶(SMZ)。所制备的ACP-PDDA-BiVO纳米片在反应60分钟后对SMR、SDZ和SMZ的去除效率达到88.9%-98.2%,并且对于SMZ降解,其动力学速率常数分别约为BiVO、PDDA-BiVO和ACP-BiVO的10倍、4.7倍和13倍。在客体-主体光催化体系中,发现ACP光敏剂在增强光吸收、促进表面电荷分离转移以及空穴(h)和超氧自由基(·O)的有效产生方面具有很大优势,极大地促进了光活性。基于鉴定出的降解中间体提出SMZ的降解途径,涉及重排、脱磺化和氧化三条主要途径。对中间体的毒性进行了评估,结果表明与母体SMZ相比,总体毒性降低。该催化剂在五次循环实验后保持92%的光催化氧化性能,并且对废水中的其他抗生素(如罗红霉素、环丙沙星等)具有共光降解能力。因此,这项工作为开发客体-主体光催化剂提供了一种简便的光敏策略,能够同时去除抗生素并有效降低废水中的生态风险。

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