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1.
Anal Chim Acta ; 1307: 342628, 2024 Jun 08.
Article in English | MEDLINE | ID: mdl-38719415

ABSTRACT

Bisphenol compounds (BPA, BPS, BPAF, etc.) are one class of the most important and widespread pollutants that poses severe threat to human health and the ecological environment. Because of the presence of multiple bisphenols in environmental and food samples, it is urgent and challenging to develop a rapid and cheap technique for simultaneously detecting BPA and its analogues. In this study, a series of M-N-C (M = Cu, Mg, Ni, Co, Fe, K) single-atom nanozymes (SAzymes) were created by simulating the structure of natural enzyme molecules, which were used as novel sensing platform for the fabrication of electrochemical sensors. Through systematic screening and characterization, it was interestingly discovered that the electrochemical sensor based on Cu-N-C SAzymes exhibited the best sensing performance for bisphenols among all SAzymes, which catalyzed not only BPA like tyrosinase, but also showed excellent catalytic capacity beyond tyrosinase (tyrosinase has no catalytic activity for BPS, BPAF, etc.), and achieved potential-resolved simultaneous rapid detection of BPA, BPS and BPAF. Further structure-activity relationship and catalytic mechanism characterizations of Cu-N-C SAzymes revealed that the presence of single atom Cu was predominantly in the form of Cu+ and Cu2+, which were anchored onto graphene nanosheet support through four coordination bonds with pyridinic N and pyrrolic N and acted as highly efficient active centers for electrocatalytic oxidation of bisphenols. The developed electrochemical sensing method exhibited excellent selectivity, sensitivity, and reliability for the rapid detection of multiple bisphenols in actual samples.


Subject(s)
Benzhydryl Compounds , Electrochemical Techniques , Phenols , Phenols/analysis , Phenols/chemistry , Benzhydryl Compounds/analysis , Electrochemical Techniques/methods , Nanostructures/chemistry , Catalysis , Copper/chemistry , Graphite/chemistry , Limit of Detection
2.
Sci Total Environ ; 924: 171383, 2024 May 10.
Article in English | MEDLINE | ID: mdl-38462003

ABSTRACT

The key to constructing an anodic electro-Fenton system hinges on two pivotal criteria: enhancing the catalyst activity and selectivity in water oxidation reaction (WOR), while simultaneously inhibiting the decomposition of hydrogen peroxide (H2O2) which is on-site electrosynthesized at the anode. To address the issues, we synthesized novel WO3/SnO2-x electrocatalysts, enriched with oxygen vacancies, capitalize on the combined activity and selectivity advantages of both WO3 and SnO2-x for the two-electron pathway electrocatalytic production of H2O2. Moreover, the introduction of oxygen vacancies plays a critical role in impeding the decomposition of H2O2. This innovative design ensures that the Faraday efficiency and yield of H2O2 are maintained at over 80 %, with a noteworthy production rate of 0.2 mmol h-1 cm-2. We constructed a novel electro-Fenton system that operates using only H2O as its feedstock and applied it to treat highly toxic uniform dimethylhydrazine (UDMH) from rocket launch effluent. Our experiments revealed a substantial total organic carbon (TOC) removal, achieving approximately 90 % after 120 mins of treatment. Additionally, the toxicity of N-nitrosodimethylamine (NDMA), a byproduct of great concern, was shown to be effectively mitigated, as evidenced by acute toxicity evaluations using zebrafish embryos. The degradation mechanism of UDMH is predominantly characterized by the advanced oxidative action of H2O2 and hydroxyl radicals, as well as by complex electron transfer processes that warrant further investigation.

3.
Environ Sci Technol ; 55(9): 6076-6086, 2021 05 04.
Article in English | MEDLINE | ID: mdl-33856783

ABSTRACT

Despite the popularity of smartphones worldwide, persistent toxic substances (PTSs) in protective cases of mobile phones (PCMPs) and their health risks via direct skin contact have been ignored. This study investigated PTSs in PCMPs made in China with different materials and sales territory and their potential harm to human health. Polybrominated diphenyl ethers (PBDEs, 6.40 ng/g), new brominated flame retardants (NBFRs, 144 ng/g), organophosphate esters (OPEs, 10.1 µg/g), short-chain chlorinated paraffins (SCCPs, 3.58 µg/g), medium-chain chlorinated paraffins (MCCPs, 3.17 µg/g), and heavy metals (HMs, 72.3 µg/g) were detected. It was found that the different concentrations and compositions depend on the material, region, and use. Moreover, the raw materials used to fabricate PCMPs are of variable quality and may include recycled plastic waste. There are no standard quality specifications for PCMPs, and different materials have different properties, including specific surface area and adsorption ability. The risk assessment performed by Monte Carlo simulations indicated that the PTSs evaluated pose no health risks to the general population and may have adverse effects on individual high-exposure populations. According to the results of this work, it is suggested that more stringent global specifications for the selection of raw materials should be established, including the content and structural characteristics of PTSs, limitations on the use of additives in the production process, and the handling after use.


Subject(s)
Cell Phone , Flame Retardants , China , Environmental Monitoring , Flame Retardants/analysis , Halogenated Diphenyl Ethers/analysis , Humans
4.
Huan Jing Ke Xue ; 40(12): 5258-5264, 2019 Dec 08.
Article in Chinese | MEDLINE | ID: mdl-31854596

ABSTRACT

In this study, samples were taken of the surface dust of main roads in Xinxiang City, and the concentrations of five heavy metals (Cd, Pb, Cr, Cu and Zn) and fifteen polycyclic aromatic hydrocarbons (PAHs) were determined by inductively coupled plasma mass spectrometry (ICP-MS) and gas chromatography-mass spectrometry (GC-MS), respectively. Meanwhile, the effects of vehicle emissions on the pollution characteristics were investigated. The results showed that the concentrations of heavy metals and PAHs ranged from 2.58 to 1560 mg·kg-1 and ND to 1.30 mg·kg-1, respectively. Overall, the concentrations of heavy metals and PAHs increased with a decrease in dust particle size. In terms of composition, the heavy metals were dominated by Zn while the high-molecular-weight PAHs were mainly homologous. In spatial distribution, the concentrations of heavy metals and PAHs were different. The total concentrations of heavy metals in road dust near Renmin Road, Xiaodian Industrial Park, and Cement Plant were the highest, while the high concentrations of PAHs appeared in the dust of Renmin Road, Upper Expressway, and 107 National Highway. Pearson correlation analysis showed that there was no positive correlation between the five heavy metals and fifteen PAHs. Then cluster analysis and factor analysis indicated that the PAHs were greatly affected by vehicle emissions, while the heavy metals were basically unaffected.

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