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通过金属-氮杂环配合物框架增强供电子策略提高氧掺杂 g-CN 的量子产率,用于高灵敏度磺胺二甲氧嘧啶追踪。

Boosting the Quantum Yield of Oxygen-Doped g-CN via a Metal-Azolate Framework-Enhanced Electron-Donating Strategy for Highly Sensitive Sulfadimethoxine Tracing.

机构信息

School of Environment, Nanjing Normal University, Wenyuan Road 1, Nanjing, Jiangsu 210023, China.

School of Food Science and Pharmaceutical Engineering, Nanjing Normal University, Nanjing, Jiangsu 210023, China.

出版信息

Anal Chem. 2022 Apr 12;94(14):5682-5689. doi: 10.1021/acs.analchem.2c00423. Epub 2022 Apr 1.

Abstract

Two of the most persistent challenges for the sensing applications of luminescent carbon nitride-based materials are poor quantum yields and aggregation-induced luminescence quenching in aqueous environments. Herein, a highly emissive oxygen-doped carbon nitride composite (OCNP@M7) was synthesized, with a metal-azolate framework (MAF-7) serving as a luminous booster. Both experimental studies and theoretical calculations suggest that the MAF-enhanced electron-donating effect dramatically promoted the electron density on the π-structure of oxygen-doped carbon nitride. In addition, the structural rigidity of MAF-7 effectively inhibits both aggregation and nonradiative energy dissipation. Consequently, OCNP@M7 exhibits strong and stable blue emission under UV light irradiation and an absolute quantum yield up to 95.2%, which is, as far as we know, the highest value among fluorescent carbon nitride materials in solution ever reported. OCNP@M7 could further function as a high-efficiency fluorescent probe for the sensitive detection of sulfadimethoxine residues in complex environments. It is anticipated that this strategy can be extended to fabricate various carbon nitride-based antibiotic monitoring systems with tailor-made functions.

摘要

对于基于发光氮化碳的传感应用,两个最持久的挑战是量子产率低和在水相环境中聚集诱导的荧光猝灭。在此,合成了一种高发光的氧掺杂氮化碳复合材料(OCNP@M7),其中金属-唑框架(MAF-7)作为发光增强剂。实验研究和理论计算都表明,MAF 增强的供电子效应显著提高了氧掺杂氮化碳的π结构上的电子密度。此外,MAF-7 的结构刚性有效地抑制了聚集和非辐射能量耗散。因此,OCNP@M7 在紫外光照射下表现出强而稳定的蓝色发射,绝对量子产率高达 95.2%,就我们所知,这是溶液中荧光氮化碳材料的最高值。OCNP@M7 可以进一步用作高效荧光探针,用于复杂环境中磺胺二甲氧嘧啶残留的灵敏检测。预计该策略可以扩展到制造具有定制功能的各种基于氮化碳的抗生素监测系统。

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