Qin Mengjie, Li Dongxue, Zhou Mengmeng, Jin Fulan, Li Yingying, Zhang Ning, Lu Minghua
Henan International Joint Laboratory of Medicinal Plants Utilization, College of Chemistry and Molecular Sciences, Henan University, Kaifeng, Henan 475004, China.
Henan International Joint Laboratory of Medicinal Plants Utilization, College of Chemistry and Molecular Sciences, Henan University, Kaifeng, Henan 475004, China.
J Hazard Mater. 2025 Sep 5;495:138952. doi: 10.1016/j.jhazmat.2025.138952. Epub 2025 Jun 15.
The utilization of an efficient and reliable coating material is of paramount importance for the effective implementation of solid-phase microextraction (SPME) process. For enhancing the adsorption capacity of metal organic framework (MOF) derived carbon materials, in this study, a series of N-doped carbon nanotubes wrapping hollow Ni-MOF-derived carbon sphere (Ni@HC-NCNTs-X) were elaborately designed and synthesized with hollow Ni-MOF as a nutritious platform and by adding dicyandiamide (DCDA) in the one-step pyrolysis processes. The mass ratios of the Ni-MOF and DCDA were optimized, and the obtained materials were used as SPME coating in conjunction with gas chromatography-tandem mass spectrometry (GC-MS/MS) for ultrasensitive determination of polychlorinated biphenyls (PCBs) from beverages. The Ni@HC-NCNTs-5 as coating material exhibited the best enrichment performance and excellent stability based on the unique hollow structure and N-doped active sites. The adsorption mechanism between Ni@HC-NCNTs-5 and PCBs was explored by combining density functional theory (DFT) calculations and experimental characterization. Under optimal conditions, the developed method possessed wide linear ranges (0.2-1000 ng L), low detection limits (0.06-0.10 ng L), and satisfactory recovery rates (71.8-115 %). The results indicated that this work provided an effective synthetic strategy for preparing adsorbents with enhanced enrichment performance for trace organic pollutants.
对于固相微萃取(SPME)过程的有效实施而言,使用高效且可靠的涂层材料至关重要。为提高金属有机框架(MOF)衍生碳材料的吸附能力,本研究精心设计并合成了一系列以空心Ni-MOF为营养平台、在一步热解过程中添加双氰胺(DCDA)制备的N掺杂碳纳米管包裹空心Ni-MOF衍生碳球(Ni@HC-NCNTs-X)。优化了Ni-MOF与DCDA的质量比,并将所得材料与气相色谱-串联质谱(GC-MS/MS)联用作为SPME涂层,用于超灵敏测定饮料中的多氯联苯(PCBs)。基于独特的空心结构和N掺杂活性位点,Ni@HC-NCNTs-5作为涂层材料表现出最佳的富集性能和出色的稳定性。通过结合密度泛函理论(DFT)计算和实验表征,探究了Ni@HC-NCNTs-5与PCBs之间的吸附机理。在最佳条件下,所建立的方法具有宽线性范围(0.2 - 1000 ng L)、低检测限(0.06 - 0.10 ng L)和令人满意的回收率(71.8 - 115%)。结果表明,这项工作为制备对痕量有机污染物具有增强富集性能的吸附剂提供了一种有效的合成策略。