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Science China-Chemistry · 2020 ·Vol. 63 ·期 4 ·554-560 · IF 6.356

In situ formation of fluorescent silicon-containing polymer dots for alkaline phosphatase activity detection and immunoassay

Liu Guoyong,Zhao Jiahui,Yan Mengxia,Zhu Shuyun,Dou Wenchao,Sun Jian,Yang Xiurong

The discovery and application of analyte-triggered fluorophore generation or fluorogenic reaction are significant and beneficial to the development of novel fluorescence (FL) analysis method. In this study, for the first time, we have reported a fluorogenic reaction to prepare fluorescent silicon-containing polymer dots (Si-PDs) by simply mixing N -[3-(trimethoxysilyl)propyl]ethylenediamine (DAMO) and hydroquinone (HQ) in aqueous solution at ambient temperature. Inspired by the alkaline phosphatase (ALP)-catalyzed hydrolysis of the substrate sodium 4-hydroxyphenyl phosphate (4-HPP) into HQ and the resultant HQ-controlled intense green Si-PDs generation, we have established a straightforward ALP activity assay by innovatively employing commercially available 4-HPP as the substrate. More significantly, the specific preparation method, clear formation mechanism and excellent performance enable the Si-PDs as well as its generation process to develop facile and attractive FL immunoassay. With the help of the universal ALP-based enzyme-linked immunosorbent assay (ELISA) platform and corresponding antibody, a convenient and conceptual ALP-based fluorescent ELISA has been constructed and applied in sensing cardiac troponin I (cTnI), a well-known biomarker of acute myocardial infarction. Our research via in situ formation of fluorescent nanomaterials has great potential application in ALP activity assay, inhibitor screening, and disease diagnosis.

CAS / MDL: 1760-24-3
研究领域: 分析化学 · 生物化学 · 纳米材料 · 诊断学 · 免疫分析
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Journal of Cleaner Production · 2023 · IF 11.1

The removal of antibiotic, antibiotic resistant bacteria and genes in persulfate oxidation system via activating by antibiotic fermentation dregs derived biochar

Yafei Wang,Chenhao Wang,Shen Yan,Yingchun Li,Chen Cai,Huiling Liu,Peng Ren,Mengmeng Wang,Shaoping Kuang

To reduce the adverse effects of antibiotics and antibiotic resistance genes (ARGs) in the environment, nitrogen-doped biochar (NLBH), derived from lincomycin fermentation dregs (LFD), was employed as an activator in a persulfate (PDS) oxidation system. The system was evaluated for its ability to degrade tetracycline (TC), inactivate antibiotic resistant bacteria (ARB) and remove ARGs. The degradation efficiency of TC in the NLBH/PDS system (70.1%) was higher than that in the pristine biochar/PDS system (10.3%). It was confirmed that the defects and edge pyridinic nitrogen generated in the nitrogen doping process were the reactive sites for PDS activation. According to electron paramagnetic resonance (EPR) and radical quenching experiments, the major mechanism for PDS activation was a non-radical pathway dominated by singlet oxygen ( 1 O 2 ). Radical pathways involving sulfate (SO 4 · - ) and hydroxyl radicals (·OH) were also at play in the NLBH/PDS system, but their role was minor. TC was principally degraded by hydroxylation , demethylation, and decarboxylation , and within 90 min, the NLBH/PDS system effectively inactivated 71.5% of ARB ( Pseudomonas sp. HLS-6). Intracellular ARGs (iARGs; sul 1, sul 2) and intI 1 had log reduction efficiencies of 2.73–4.04 and 2.70, respectively, whereas, extracellular ARGs ( sul 1 and sul 2) and intI 1 accumulated noticeably by 1.52–4.18-and 4.92-log, respectively. This work highlights a promising alternative technique for the removal of antibiotics, ARB and iARGs in future advanced wastewater treatment systems.

CAS / MDL: 7727-21-1
研究领域: 环境科学 · 化学工程 · 微生物学 · 废物管理
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WATER RESEARCH · 2024 · IF 11.4

Molecular-level transformations of dissolved black carbon in UV-based advanced oxidation processes

Qi Lu,Qi Han,Hongnan Liu,Li Feng,Yongze Liu,Ziwen Du,Liqiu Zhang

Dissolved black carbon (DBC) released from biochar, is an essential group in the dissolved organic matter (DOM) pool and is widely distributed in aquatic environments. In various advanced oxidation processes (AOPs), DBC exhibits enhanced free radical scavenging compared to typical DOM, attributed to its smaller molecular weight and more compacted aromatic structure; however, the molecular-level transformations of DBC in different AOPs , such as UV/H 2 O 2 , UV/PDS, and UV/Chlorine, remain unclear. This study employed a DBC derived from wheat biochar for experimentation. Characterization involved ultraviolet-visible (UV–Vis) spectroscopy and fluorescence excitation-emission-matrix (EEM) spectroscopy, revealing the transformation of DBC through diminished SUVA 254 values and reduced intensity of three-dimensional fluorescence peaks. Further insights into the transformation were gained through Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS). After each UV-AOP treatment, a conspicuous augmentation in the oxygen content of DBC was observed. The detailed oxygenation processes were elucidated through mass difference analysis, based on 23 types of typical reactions. Results indicated that oxygenation reactions were most frequently detected in all three UV-AOP treatments. Specifically, the hydroxylation (+O) predominated in UV/H 2 O 2 , while the di-hydroxylation (+2O) prevailed in UV/PDS. UV/Chlorine treatments commonly exhibited tri-hydroxylation (+3O), with the identification of 1194 Cl-BPs of unknown structures. This study contributes to a comprehensive understanding of the molecular transformations of DBC induced by various free radicals in different UV-AOP processes, leading to a better understanding of the different fates of DBC in UV-AOP processes. In addition, the identification of DBC as a precursor of by-products will also contribute to the understanding of how to inhibit the generation of by-products.

研究领域: 环境科学 · 化学工程 · 分析化学 · 水处理
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