Science of the Total Environment ( IF 8.2 ) Pub Date : 2022-07-19 , DOI: 10.1016/j.scitotenv.2022.157470 Yi-Fan Wang 1 , Zhi Li 1 , Ming Jiang 1 , Xu Yu 1 , Li Xu 1
Detection and removal of contaminants are significant for environmental monitoring and remediation. In the present study, “two-in-one” silicon nanoparticles (SiNPs) were designed and prepared to simultaneously act as the fluorescent probe and degradation catalyst to detect and remove tetracycline (TCs) antibiotics. Thiourea and 3-aminopropyltrimethoxysilane were dopant and silicon source to generate fluorescent sulfur and nitrogen co-doped SiNPs (SN-SiNPs). The blue fluorescence of SN-SiNPs was selectively quenched by TCs due to the inner filter effect, whilst accompanied by the newly appeared yellow-green fluorescence resulting from aggregation induced fluorescence emission effect. Based on this phenomenon, SN-SiNPs can be used as fluorescent colorimetric probes for detection of doxycycline, oxytetracycline and tetracycline with limits of detection of 1.8 μg/L, 3.0 μg/L and 4.2 μg/L, respectively; the semi-quantitation can even be visually achieved by naked eyes. Particularly, SN-SiNPs were capable to catalyze the degradation of the three TCs effectively, achieving the removal rates of doxycycline, oxytetracycline and tetracycline of >90 %, >80 % and > 70 % after 240 min exposure to UV light. The catalytic ability of SN-SiNPs was derived from hydroxyl radical (•OH−), superoxide radical (•O2−) and singlet oxygen (1O2) produced by SN-SiNPs under UV irradiation. Moreover, integrating the fluorescent probe and photocatalyst together, the proposed SN-SiNPs simultaneously realized catalyzing the degradation of the three TCs and in-situ visually monitoring of the degradation process in real time. This study innovatively proposed an integrated probe for the detection and catalytic degradation of TCs, providing a new “two-in-one” strategy for rapid and simple detection and removal of drug pollutants.
中文翻译:
“二合一”硫氮共掺杂荧光硅纳米粒子:同时作为荧光探针和光催化剂用于原位实时视觉监测和降解四环素类抗生素
污染物的检测和去除对于环境监测和修复具有重要意义。在本研究中,设计和制备了“二合一”硅纳米粒子(SiNPs),同时作为荧光探针和降解催化剂,检测和去除四环素(TCs)抗生素。硫脲和 3-氨基丙基三甲氧基硅烷是掺杂剂和硅源以产生荧光硫和氮共掺杂的 SiNPs (SN-SiNPs)。SN-SiNPs的蓝色荧光由于内部过滤效应而被TCs选择性猝灭,同时伴随着由聚集诱导的荧光发射效应产生的新出现的黄绿色荧光。基于这一现象,SN-SiNPs可以作为荧光比色探针用于检测强力霉素,土霉素和四环素的检测限分别为 1.8 μg/L、3.0 μg/L 和 4.2 μg/L;半定量甚至可以通过肉眼目测实现。特别是,SN-SiNPs能够有效催化三种TCs的降解,在紫外光照射240分钟后,多西环素、土霉素和四环素的去除率分别为>90%、>80%和>70%。SN-SiNPs 的催化能力来源于羟基自由基 (•OH− )、超氧自由基 (•O 2 − ) 和单线态氧 ( 1 O 2 ) 由 SN-SiNPs 在紫外线照射下产生。此外,将荧光探针和光催化剂集成在一起,所提出的SN-SiNPs同时实现了催化三种TCs的降解和实时原位视觉监测降解过程。本研究创新性地提出了一种用于TCs检测和催化降解的集成探针,为快速简便地检测和去除药物污染物提供了一种新的“二合一”策略。