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Luminescent 2D Pillared-Bilayer Metal–Organic Coordination Networks for Selective Sensing of ReO4– in Water
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2021-09-16 , DOI: 10.1021/acsami.1c11606 Sheeba Khan 1 , Sanjay K Mandal 1
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2021-09-16 , DOI: 10.1021/acsami.1c11606 Sheeba Khan 1 , Sanjay K Mandal 1
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For the preference in nuclear energy, one of the high-level liquid waste materials in the form of pertechnetate anion (TcO4–) has become an environmental hazard due to its mobility into groundwater and soil. For its sequestration, numerous efforts have been reported in recent years. However, its selective sensing, even using its nonradioactive surrogate oxidizing perrhenate ion (ReO4–), in aqueous media is very limited. To develop novel materials for such a purpose, we have designed an amino acid-functionalized bent dicarboxylic acid, 4-(((4-((carboxymethyl)carbamoyl)phenyl)amino)methyl)benzoic acid (H2hipamifba), for the strategic room-temperature synthesis of two isostructural and highly luminescent two-dimensional (2D) metal–organic coordination networks (MOCNs), {[Cu(hipamifba)(4,4′-azbpy)]·2CH3OH·2H2O}n (1) and {[Zn(hipamifba)(4,4′-azbpy)]·2CH3OH·2H2O}n (2), where 4,4′-azobipyridine (4,4′-azbpy) as a pillar linker imparts luminescent properties in the architectures. The single-crystal X-ray structural analysis demonstrates that 1 and 2 have pillared-bilayer 2D networks with the sq1/Shubnikov tetragonal plane net topology. These multiresponsive luminescent materials were gainfully employed for the selective sensing of ReO4– in water with a detection limit of 3.4 and 5.4 ppm for 1 and 2, respectively. It is noteworthy to point out that these are the first neutral sensors for such study as the only other two sensors reported in the literature are cationic in nature. Their suitability (selectivity, stability, and recyclability) as excellent water-stable sensors was established through the competitive analyte test and a comparison of pristine and spent samples by powder X-ray diffraction (PXRD) and scanning electron microscopy (SEM). Further, the mechanism of selective detection is explained by the time-resolved studies and density functional theory (DFT) calculations.
中文翻译：
用于选择性检测水中 ReO4– 的发光二维柱状双层金属-有机配位网络
出于对核能的偏好，高锝酸阴离子 (TcO 4 – )形式的一种高放液态废物因其可迁移到地下水和土壤中而成为一种环境危害。对于它的封存，近年来已经报道了许多努力。然而，它的选择性传感，即使使用其非放射性替代氧化高铼酸离子 (ReO 4 – )，在水性介质中也非常有限。为了开发用于此目的的新材料，我们设计了一种氨基酸官能化的弯曲二羧酸，4-(((4-((羧甲基)氨基甲酰基)苯基)氨基)甲基)苯甲酸 (H 2hipamifba)，用于战略性室温合成两种同构和高发光二维 (2D) 金属-有机配位网络 (MOCN)，{[Cu(hipamifba)(4,4'-azbpy)]·2CH 3 OH ·2H 2 O} n ( 1 ) 和{[Zn(hipamifba)(4,4'-azbpy)]·2CH 3 OH·2H 2 O} n ( 2 )，其中4,4'-偶氮联吡啶(4,4 '-azbpy) 作为支柱连接器赋予结构中的发光特性。单晶 X 射线结构分析表明1和2具有带 sq1/Shubnikov 四方平面网络拓扑结构的柱状双层 2D 网络。这些多响应发光材料被有效地用于 ReO 4的选择性传感-在水中，1和2的检测限分别为 3.4 和 5.4 ppm， 分别。值得注意的是，这些是用于此类研究的第一个中性传感器，因为文献中报道的其他两种传感器本质上是阳离子。通过竞争性分析物测试以及通过粉末 X 射线衍射 (PXRD) 和扫描电子显微镜 (SEM) 对原始样品和废样品进行比较，确定了它们作为出色的水稳定性传感器的适用性（选择性、稳定性和可回收性）。此外，选择性检测的机制可以通过时间分辨研究和密度泛函理论 (DFT) 计算来解释。
更新日期：2021-09-29
中文翻译：
用于选择性检测水中 ReO4– 的发光二维柱状双层金属-有机配位网络
出于对核能的偏好，高锝酸阴离子 (TcO 4 – )形式的一种高放液态废物因其可迁移到地下水和土壤中而成为一种环境危害。对于它的封存，近年来已经报道了许多努力。然而，它的选择性传感，即使使用其非放射性替代氧化高铼酸离子 (ReO 4 – )，在水性介质中也非常有限。为了开发用于此目的的新材料，我们设计了一种氨基酸官能化的弯曲二羧酸，4-(((4-((羧甲基)氨基甲酰基)苯基)氨基)甲基)苯甲酸 (H 2hipamifba)，用于战略性室温合成两种同构和高发光二维 (2D) 金属-有机配位网络 (MOCN)，{[Cu(hipamifba)(4,4'-azbpy)]·2CH 3 OH ·2H 2 O} n ( 1 ) 和{[Zn(hipamifba)(4,4'-azbpy)]·2CH 3 OH·2H 2 O} n ( 2 )，其中4,4'-偶氮联吡啶(4,4 '-azbpy) 作为支柱连接器赋予结构中的发光特性。单晶 X 射线结构分析表明1和2具有带 sq1/Shubnikov 四方平面网络拓扑结构的柱状双层 2D 网络。这些多响应发光材料被有效地用于 ReO 4的选择性传感-在水中，1和2的检测限分别为 3.4 和 5.4 ppm， 分别。值得注意的是，这些是用于此类研究的第一个中性传感器，因为文献中报道的其他两种传感器本质上是阳离子。通过竞争性分析物测试以及通过粉末 X 射线衍射 (PXRD) 和扫描电子显微镜 (SEM) 对原始样品和废样品进行比较，确定了它们作为出色的水稳定性传感器的适用性（选择性、稳定性和可回收性）。此外，选择性检测的机制可以通过时间分辨研究和密度泛函理论 (DFT) 计算来解释。
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