A 3D hierarchical dual-metal–organic framework heterostructure up-regulating the pre-concentration effect for ultrasensitive fluorescence detection of tetracycline antibiotics,Journal of Materials Chemistry C

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A 3D hierarchical dual-metal–organic framework heterostructure up-regulating the pre-concentration effect for ultrasensitive fluorescence detection of tetracycline antibiotics
Journal of Materials Chemistry C ( IF 5.7 ) Pub Date : 2019/12/24 , DOI: 10.1039/c9tc05941e
Chunhua Li _{1,

2,

3,

4} , Weixia Yang _{1,

2,

3,

4} , Xiaoshuo Zhang _{1,

2,

3,

4} , Yong Han _{1,

2,

3,

4} , Wenzhi Tang _{1,

2,

3,

4} , Tianli Yue _{1,

2,

3,

4,

5} , Zhonghong Li _{1,

2,

3,

4,

5}

Affiliation

Tetracycline antibiotic (TC) residues, such as doxycycline (DOX), tetracycline (TET), oxytetracycline (OTC) and chlortetracycline (CTC), have aroused public concerns due to their negative impact on human health and the ecological system. Herein, a 3D hierarchical dual-metal–organic framework, an Al-MOF@Mo/Zn-MOF heterostructure, is developed via an internal extended growth method for exceptionally high performance detection of TCs. The modified organic ligands with intriguing functional groups (–NH₂) exhibit specific recognition toward TCs, which makes the fluorescence of Al-MOF@Mo/Zn-MOF efficiently quenched by TCs via the synergistic effect of H-bonding interaction enhancing the electron transfer from –NH₂ on organic ligands to –CO–/–OH of TCs and the intense absorption of TCs at the excitation energy of Al-MOF@Mo/Zn-MOF. Particularly, the pre-concentration effect, induced by (i) metal nodes in dual-metal–organic frameworks providing unsaturated sites to recognize/adsorb the N and O atoms of TC molecules and (ii) the hierarchical nanoarchitecture enhancing mass transfer and alleviating the diffusion barrier to increase the contact area of MOF/TCs, endows Al-MOF@Mo/Zn-MOF with superior sensitivity. The Al-MOF@Mo/Zn-MOF reveals excellent anti-interference performances and ultra-low limits of detection (LODs) of 0.56, 0.53, 0.58 and 0.86 nM for DOX, TET, OTC and CTC. These acquired LOD values are two orders of magnitude lower than that of pristine amino-functionalized Al-MOF and comparable or even superior to those of previous fluorescence-based sensors. Satisfactory recoveries of 87.07–116.44% and RSDs of 0.22–2.30% are achieved in the detection of TCs in real water and food samples. These excellent sensing properties together with the advantages of facile fabrication, satisfactory stability and feasibility render the 3D hierarchical Al-MOF@Mo/Zn-MOF heterostructure promising for ultrasensitive detection of TCs in practical applications.

中文翻译：

3D分层双金属-有机框架异质结构上调了四环素抗生素超灵敏荧光检测的预富集效应

四环素抗生素（TC）残留物，例如强力霉素（DOX），四环素（TET），土霉素（OTC）和金霉素（CTC），由于其对人体健康和生态系统的负面影响而引起了公众的关注。在这里，通过内部扩展生长方法开发了3D分层双金属有机框架Al-MOF @ Mo / Zn-MOF异质结构，用于TC的异常高性能检测。具有有趣的官能团（–NH ₂）的改性有机配体对TC表现出特异性识别，这使得Al-MOF @ Mo / Zn-MOF的荧光通过H键相互作用的协同作用增强了电子传递，从而被TC有效地猝灭了。来自–NH ₂对TCs –CO – / – OH的有机配体具有一定的吸附作用，并且在Al-MOF @ Mo / Zn-MOF的激发能下TCs的强烈吸收。尤其是，预浓缩效应是由（i）双金属有机框架中的金属节点提供不饱和的位点来识别/吸附TC分子的N和O原子，以及（ii）分层的纳米结构增强了质量转移并减轻了扩散阻挡层可增加MOF / TC的接触面积，赋予Al-MOF @ Mo / Zn-MOF优异的灵敏度。Al-MOF @ Mo / Zn-MOF具有出色的抗干扰性能，并且DOX，TET，OTC和CTC的检测限（LOD）分别为0.56、0.53、0.58和0.86 nM。这些获得的LOD值比原始氨基官能化的Al-MOF低两个数量级，并且与以前的基于荧光的传感器相当或什至更好。在真实水和食品样品中检测TC时，回收率令人满意，为87.07–116.44％，RSD为0.22–2.30％。这些出色的感测特性以及易于制造，令人满意的稳定性和可行性的优点，使3D分层Al-MOF @ Mo / Zn-MOF异质结构有望在实际应用中用于TC的超灵敏检测。

更新日期：2020-02-13

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