MOLECULES
·
2022
·Vol. 27
·期 20
·7064
·
IF 4.927
Jia Liu,Chao Ding,Sicheng Gong,Kun Fu,Huiping Deng,Jun Shi
The nonradical process in the peroxydisulfate (PDS) oxidation system is a promising method for antibiotic removal in water. In this study, CuO@CNT was successfully synthesized by a facile approach to catalyze PDS. The removal efficiency of the antibiotic sulfamethoxazole (SMX) was 90.6% in 50 min, and the stoichiometric efficiency (ΔSMX/ΔPDS) was 0.402. The very different degradation efficiency of common organic contaminants revealed the selective oxidation of the surveyed system. The process of1O2oxidation and the electron-transfer regime was exhibited by chemical quenching tests, electron paramagnetic resonance (EPR) determination, a UV–vis spectrophotometer, X-ray photoelectron spectroscopy (XPS) detection, and cyclic voltammetry (CV) measurements. Sustainable catalysis was promoted by the circulation between the surface electron-rich centers of Cu(II) and Cu(III). Dissolved oxygen (DO) and a metastable Cu(III) intermediate contributed to the generation of1O2. Still, a portion of SMX was removed by the mildly activated PDS. Moreover, the influence factors (pH, dosage, water matrix) were examined, and suppressions were acceptable by common anions and real water. Distinguished from the radical process, unique intermediate products were ascertained via the theoretical calculation and liquid chromatography–mass spectrometry (LC-MS) detection. Furthermore, CuO@CNT showed a satisfactory activation ability in the cycling experiments. Overall, this study developed CNT to be a supporter of CuO, unveiled the mechanism of catalysis, and evaluated the application potential of the nonradical process.Keywords:peroxydisulfate;nonradical process;singlet oxygen;trivalent copper;electron transfer
研究领域:
环境科学
·
化学
✓ 已验证
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Hui Hong,Minghao Xu,Xuerui Yang,Lei Zhou,Jean-Marc Chovelon,Guangli Xiu
Copper-based catalysts have been widely used in heterogeneous advanced oxidation processes (AOPs) to degrade emerging contaminants, with trivalent copper species (Cu(III)) often identified as crucial intermediates. However, the current understanding of the reactivity and potential oxidation mechanism associated with such reactive species remains quite limited. In the present study, a stable Cu(III) complex was synthesized, and its reactivity towards a typical fluoroquinolone antibiotic, ofloxacin (OFX), was comprehensively investigated. The results revealed that Cu(III) itself functioned as the primary oxidizing agent instead of secondary hydroxyl radicals generated during OFX decomposition, which exhibited high reactivity over a wide pH range (3.0–9.0) with molar ratio of Cu(III) to OFX between 1:2 and 3:1. Interestingly, prevalent constituents of natural water, including (bi)carbonate (0–10 mM), chloride (0–10 mM), nitrate (0–10 mM) and humic acid (0–30 mg/L), displayed minimal influence on the oxidation efficiency of Cu(III). Piperazine moiety was identified as the primary reaction site, and three different pathways including tertiary amine oxidation, hydroxylation, and N-demethylation process were proposed. The detailed oxidation mechanisms were further illustrated by density functional theory (DFT) calculations. This study contributes to the theoretical foundation for investigating the mechanism of Cu(III)-mediated oxidation of antibiotics.
研究领域:
环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
ELECTROPHORESIS
·
2012
·Vol. 33
·期 11
·1589-1594
·
IF 3.303
Lin Wang,Ying Liu,Haoyue Xie,Zhifeng Fu
A transition metal chelate unstable at a high oxidation state, diperiodatocuprate (III) (K 5 [Cu(HIO 6 ) 2 ], DPC), was synthesized and applied in the luminol-based chemiluminescence (CL) system for highly sensitive CE end-column detection of dopamine (DA). This method was based on the fact that DA enhanced the CL emission resulting from the reaction between luminol and DPC in alkaline medium. The DPC-luminol-DA CL system showed very intensive emission and very fast kinetic characteristics, thus resulting in a high sensitivity in flow-through detection mode for CE. Under optimal conditions, the linear range was 1.0 × 10 −8 –5.0 × 10 −5 g/mL ( R 2 = 0.9984) with a limit of detection of 6.0 × 10 −9 g/mL (S/N = 3). The RSDs of the peak height and the migration time were about 4.2 and 2.4% for a standard sample at 3.0 × 10 −6 g/mL ( n = 5), respectively. The presented method has been successfully used for the determination of DA in commercial preparation and human urine samples after clean-up using SPE.
研究领域:
分析化学
·
生物医学
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DOI
PubMed
高影响因子
ANALYTICA CHIMICA ACTA
·
2012
·
IF 4.555
Tao Li,Haoyue Xie,Zhifeng Fu
A facile, sensitive and universal method was established for analysis of biogenic amines using micellar electrokinetic chromatography coupled with chemiluminescent (CL) detection. It was found that diperiodatocuprate (III) (K 5 [Cu(HIO 6 ) 2 ], DPC), a transition metal chelate at unstable high oxidation state, could effectively enhance the reaction between luminol-type compound and hydrogen peroxide, to produce very strong CL signal. In addition, triethylamine was found to be able to effectively improve the yield of the derivatization reaction between biogenic amines and a luminol-type derivatization reagent, N -(4-aminobutyl)- N -ethylisoluminol (ABEI). Based on these facts, three biogenic amines were pre-column derivatized with ABEI, and post-column detected using high sensitive luminol-hydrogen peroxide-DPC CL system. Since the background was quite low, and the signal was quite strong, a considerable improved sensitivity was obtained. The presented method had been successfully applied to simultaneously analyze glycine, proline and phenylalanine with the detection limits (S/N = 3) of 0.030 μmol L −1 , 0.23 μmol L −1 and 0.21 μmol L −1 , respectively. To evaluate its potential application value, glycine in saliva and urine samples was detected using this method, and satisfied results were obtained. This approach can be further extended to detection of many other compounds such as peptides and drugs by using luminol-type derivatization reagent.
研究领域:
分析化学
·
生物化学
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DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Hengxin Liu,Haoxi Dai,Shuang Wu,Ning Li,Beibei Yan,Guanyi Chen
Persulfate (PS) activated by thermal or homogeneous metals can generate reactive oxygen species (ROS) and high-valence-state metals for contaminants degradation, showing great potential for applications. However, thermal effect in peroxymonosulfate (PMS) system with high-valence-state metal is still ambiguous. In this study, divalent copper (Cu(II)) catalysis was taken to explore thermal effect on PMS performance. Results showed that the Sulfamethoxazole (SMX) removal efficiency in the Cu(II)/PMS system at 60 min increased by only 5.9% with temperature increase from 30 °C to 60 °C. Moreover, SMX removal efficiency was excellent at neutral or basic pH, best with PMS concentration of 2.4 mM, and slightly affected by Cu(II) concentration. The singlet oxygen ( 1 O 2 ) was identified as main active species at low temperature while sulfate radicals (SO 4 − ) was more effective at high temperature with Cu(II) co-activation. Also, trivalent copper (Cu(III)) was an important active species. The higher Cu(III) content, the better SMX removal efficiency, but the stronger intermediates toxicity. In combination with removal efficiency and intermediates toxicity at different temperatures, 30 °C was the optimal reaction temperature. Overall, this study provides new perspective on utilization of waste heat and high-valence-state metal for organic wastewater treatment in PMS systems.
研究领域:
环境科学
·
化学工程
·
水处理
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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