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Tailor-Made Multiple Interpenetrated Metal–Organic Framework for Selective Detection and Adsorption of ReO4–
Analytical Chemistry ( IF 6.7 ) Pub Date : 2022-11-17 , DOI: 10.1021/acs.analchem.2c03983 Qing-Hua Hu 1 , Xin Gao 1 , Yu-Zhen Shi 1 , Ru-Ping Liang 1 , Li Zhang 1 , Sen Lin 1 , Jian-Ding Qiu 1, 2
Analytical Chemistry ( IF 6.7 ) Pub Date : 2022-11-17 , DOI: 10.1021/acs.analchem.2c03983 Qing-Hua Hu 1 , Xin Gao 1 , Yu-Zhen Shi 1 , Ru-Ping Liang 1 , Li Zhang 1 , Sen Lin 1 , Jian-Ding Qiu 1, 2
Affiliation
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Rationally designed new materials for the selective detection and adsorption of 99Tc, a problematic element in nuclear waste, are important and challenging in environmental monitoring. Here, we utilize an interpenetration approach to develop a cationic fluorescent metal–organic framework (NCU-2), which was constructed by a flexible tridentate nitrogen-containing ligand and Ag+ metal ions. The NCU-2 is a scarce case of 14-fold interpenetrated with excellent chemical stability even under 0.5 M HNO3, which is helpful for the detection and removal of ReO4–/TcO4– from nuclear waste. Excitingly, the fluorescence signal of NCU-2 was obviously quenched in the presence of ReO4– (a nonradioactive surrogate of TcO4–) due to the robust interaction between ReO4– and the host for the formation of a non-fluorescent complex. Furthermore, the NCU-2 exhibits a high selectivity sensing of ReO4– in the presence of excess competitive ions. The superior response of NCU-2 toward ReO4– is ascribed to the high-fold structure and the luxuriant unsaturated Ag metal sites on the wall of 1D pore channels, which can enhance the framework positive charge and accelerate the transport of guest molecules to strengthen the interaction between them. Notably, NCU-2 successfully quantified trace levels of ReO4– in simulated Hanford waste with a broad linear range (0.2–200 μM) and a low detection limit of 66.7 nM. Moreover, NCU-2 also shows a high adsorption capacity to ReO4– (541 mg/g) and rapid sorption kinetics, making it extremely attractive for waste monitoring and emergency remediation.
中文翻译：
用于 ReO4 选择性检测和吸附的定制多重互穿金属-有机框架-
合理设计用于选择性检测和吸附99 Tc（核废料中的问题元素）的新材料在环境监测中具有重要和挑战性。在这里，我们利用互穿方法开发了一种阳离子荧光金属有机骨架 (NCU-2)，它由柔性三齿含氮配体和 Ag +金属离子构成。NCU-2是稀有的14重互穿结构，即使在0.5 M HNO 3下也具有优异的化学稳定性，有助于检测和去除核废料中的ReO 4 – /TcO 4 – 。令人兴奋的是，NCU-2 的荧光信号在 ReO 4存在下明显猝灭–（TcO 4的非放射性替代品–）由于 ReO 4 –与主体之间的强烈相互作用，形成了非荧光复合物。此外，NCU - 2在存在过量竞争离子的情况下表现出对 ReO 4的高选择性感测。NCU-2对ReO 4的优异响应归因于高折叠结构和一维孔道壁上丰富的不饱和Ag金属位点，可以增强框架正电荷并加速客体分子的传输以增强他们之间的互动。值得注意的是，NCU-2 成功量化了 ReO 4的痕量水平–在具有宽线性范围 (0.2–200 μM) 和 66.7 nM 的低检测限的模拟汉福德废物中。此外，NCU-2 还显示出对 ReO 4 – (541 mg/g)的高吸附能力和快速吸附动力学，使其在废物监测和紧急修复方面极具吸引力。
更新日期：2022-11-17
中文翻译：
用于 ReO4 选择性检测和吸附的定制多重互穿金属-有机框架-
合理设计用于选择性检测和吸附99 Tc（核废料中的问题元素）的新材料在环境监测中具有重要和挑战性。在这里，我们利用互穿方法开发了一种阳离子荧光金属有机骨架 (NCU-2)，它由柔性三齿含氮配体和 Ag +金属离子构成。NCU-2是稀有的14重互穿结构，即使在0.5 M HNO 3下也具有优异的化学稳定性，有助于检测和去除核废料中的ReO 4 – /TcO 4 – 。令人兴奋的是，NCU-2 的荧光信号在 ReO 4存在下明显猝灭–（TcO 4的非放射性替代品–）由于 ReO 4 –与主体之间的强烈相互作用，形成了非荧光复合物。此外，NCU - 2在存在过量竞争离子的情况下表现出对 ReO 4的高选择性感测。NCU-2对ReO 4的优异响应归因于高折叠结构和一维孔道壁上丰富的不饱和Ag金属位点，可以增强框架正电荷并加速客体分子的传输以增强他们之间的互动。值得注意的是，NCU-2 成功量化了 ReO 4的痕量水平–在具有宽线性范围 (0.2–200 μM) 和 66.7 nM 的低检测限的模拟汉福德废物中。此外，NCU-2 还显示出对 ReO 4 – (541 mg/g)的高吸附能力和快速吸附动力学，使其在废物监测和紧急修复方面极具吸引力。
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