pH 值高度稳定的稀土 MOF：磺胺二甲嘧啶的可调发光和比率发光探针,Dalton Transactions

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pH 值高度稳定的稀土 MOF：磺胺二甲嘧啶的可调发光和比率发光探针
Dalton Transactions ( IF 3.5 ) Pub Date : 2023-05-18 , DOI: 10.1039/d3dt01117h
Xu Zhang ₁ , Dongyan Liu ₁ , Jiahui Yu ₁ , Xin Li ₁ , Hanwen Zheng ₁ , Yanan Zhou ₁ , Cuiying Huang ₁ , Yanyu Zhu ₁ , Chengqi Jiao _{1,

2} , Zhengang Sun ₁

Affiliation

通过选择双膦酸配体 H ₄ L (H ₄ L = 4-FC ₆ H ₄ CH ₂ N(CH ₂ PO ₃ H ₂ ) ₂ ) 和共配体草酸盐 (H ₂ C ₂ O ₄ )，三种同构镧系金属–具有二维层状结构的有机框架（Ln-MOF），[Ln(H ₃ L)(C ₂ O ₄ )]·2H ₂ O（Ln = Eu ( 1 )、Gd ( 2 ) 或 Tb ( 3 )），通过水热法制备。^{通过调节Eu 3+}、Gd的摩尔比上述反应中的³⁺和 Tb^{3+ 、六种双金属或三金属掺杂的 Ln-MOF (Eu}_x Tb_{1− x} ( x = 0.02 ( 4 ) 、 0.04 ( 5 ) 和 0.06 ( 6 ) )、Gd_0.94 Eu获得_0.06 ( 7 )、Gd_0.96 Tb_0.04 ( 8 )和Gd_0.95 Tb_0.03 Eu_0.02 ( 9 ))。掺杂Ln-MOFs 4-9的粉末X射线衍射（PXRD）图表明它们与1-3是同晶的。双金属掺杂的Ln-MOFs的发光颜色在黄绿色、黄色、橙色、粉色和浅蓝色之间逐渐变化。同时，三金属掺杂的Gd _0.95 Tb _0.03 Eu _0.02 Ln-MOF( 9 )显示出近白光发射，量子产率为11.39%。有趣的是， 1-9的夜光油墨是不可见的且颜色可调，这使得推广其防伪应用成为可能。此外，3表现出良好的热稳定性、水稳定性和pH稳定性，这为其传感应用提供了可行性。发光传感实验表明3可作为磺胺二甲嘧啶 (SMZ) 的高选择性、可重复使用和比率发光传感器。此外，3在真实样品（例如海水养殖水和真实尿液）中表现出优异的SMZ检测性能。由于紫外灯下响应信号的明显变化，制备了便携式SMZ试纸。

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Highly pH-stable lanthanide MOFs: a tunable luminescence and ratiometric luminescent probe for sulfamethazine

By selecting a bisphosphonic ligand H₄L (H₄L = 4-F-C₆H₄CH₂N(CH₂PO₃H₂)₂) and a coligand oxalate (H₂C₂O₄), three isostructural lanthanide metal–organic frameworks (Ln-MOFs) with a 2D layer structure, [Ln(H₃L)(C₂O₄)]·2H₂O (Ln = Eu (1), Gd (2), or Tb (3)), were hydrothermally prepared. By tuning the molar ratio of Eu³⁺, Gd³⁺, and Tb³⁺ in the above reactions, six bimetallic or trimetallic doped Ln-MOFs (Eu_xTb_1−x (x = 0.02 (4), 0.04 (5), and 0.06 (6)), Gd_0.94Eu_0.06 (7), Gd_0.96Tb_0.04 (8) and Gd_0.95Tb_0.03Eu_0.02 (9)) were obtained. The powder X-ray diffraction (PXRD) patterns of doped Ln-MOFs 4–9 show that they are isomorphous with 1–3. The bimetallic doped Ln-MOFs show a gradual variation of luminous colors between yellow-green, yellow, orange, pink, and light blue. Meanwhile, the trimetallic doped Gd_0.95Tb_0.03Eu_0.02 Ln-MOF (9) displays near white-light emission with a quantum yield of 11.39%. Interestingly, the luminous inks of 1–9 are invisible and color tunable, which makes it possible to promote their anti-counterfeiting applications. Additionally, 3 displays good thermal, water, and pH stabilities, which provides the feasibility for its sensing application. The luminescence sensing experiments show that 3 can serve as a highly selective, reusable, and ratiometric luminescent sensor of sulfamethazine (SMZ). Moreover, 3 shows an excellent SMZ detection performance in real samples, such as mariculture water and real urine. Owing to the visible variation of the response signal under a UV lamp, portable SMZ test paper was prepared.

更新日期：2023-05-18

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