Highly selective and sensitive detection of Hg2+ by a novel fluorescent probe with dual recognition sites

Li, Hongqi; Li, Jiayin; Pan, Zhixiu; Zheng, Tao; Song, Yanxi; Zhang, Jian; Xiao, Zhongwen

doi:10.1016/j.saa.2023.122379

Cited by 14 publications

(4 citation statements)

References 67 publications

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“…These results further support the hypothesis that the 197m/g Hg 2+ may coordinate through the isothiocyanate at the radiolabeling scale. However, radiolabeling was still achieved in the presence of the sulfur containing thiourea, as these functional groups have also been documented in the literature to coordinate Hg 2+ ( Lin et al, 2010 ; Olsen et al, 2015 ; Li et al, 2023 ).…”

Section: Resultsmentioning

confidence: 99%

Exploration of commercial cyclen-based chelators for mercury-197 m/g incorporation into theranostic radiopharmaceuticals

Randhawa,

Carbo-Bague,

Davey

et al. 2024

Front. Chem.

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A comprehensive investigation of the Hg2+ coordination chemistry and 197m/gHg radiolabeling capabilities of cyclen-based commercial chelators, namely, DOTA and DOTAM (aka TCMC), along with their bifunctional counterparts, p-SCN-Bn-DOTA and p-SCN-Bn-TCMC, was conducted to assess the suitability of these frameworks as bifunctional chelators for the 197m/gHg2+ theranostic pair. Radiolabeling studies revealed that TCMC and DOTA exhibited low radiochemical yields (0%–6%), even when subjected to harsh conditions (80°C) and high ligand concentrations (10–4 M). In contrast, p-SCN-Bn-TCMC and p-SCN-Bn-DOTA demonstrated significantly higher 197m/gHg radiochemical yields (100% ± 0.0% and 70.9% ± 1.1%, respectively) under the same conditions. The [197 m/gHg]Hg-p-SCN-Bn-TCMC complex was kinetically inert when challenged against human serum and glutathione. To understand the differences in labeling between the commercial chelators and their bifunctional counterparts, non-radioactive natHg2+ complexes were assessed using NMR spectroscopy and DFT calculations. The NMR spectra of Hg-TCMC and Hg-p-SCN-Bn-TCMC suggested binding of the Hg2+ ion through the cyclen backbone framework. DFT studies indicated that binding of the Hg2+ ion within the backbone forms a thermodynamically stable product. However, competition can form between isothiocyanate binding and binding through the macrocycle, which was experimentally observed. The isothiocyanate bound coordination product was dominant at the radiochemical scale as, in comparison, the macrocycle bound product was seen at the NMR scale, agreeing with the DFT result. Furthermore, a bioconjugate of TCMC (TCMC-PSMA) targeting prostate-specific membrane antigen was synthesized and radiolabeled, resulting in an apparent molar activity of 0.089 MBq/nmol. However, the complex demonstrated significant degradation over 24 h when exposed to human serum and glutathione. Subsequently, cell binding assays were conducted, revealing a Ki value ranging from 19.0 to 19.6 nM. This research provides crucial insight into the effectiveness of current commercial chelators in the context of 197m/gHg2+ radiolabeling. It underscores the necessity for the development of specific and customized chelators to these unique “soft” radiometals to advance 197m/gHg2+ radiopharmaceuticals.

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Section: Resultsmentioning

confidence: 99%

Exploration of commercial cyclen-based chelators for mercury-197 m/g incorporation into theranostic radiopharmaceuticals

Randhawa,

Carbo-Bague,

Davey

et al. 2024

Front. Chem.

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“…Fluorescent probe sensing technology has been widely used in the detection of Hg 2+ in the environment and organisms due to its advantages of simple fabrication method, easy operation and and biologically non-destructive in situ imaging [17][18][19][20][21] . As shown in Table S1, according to the recognition mechanism of Hg 2+ , it can be mainly divided into two types of uorescent probes: complexation probes [22][23][24] and reaction probes [25][26][27] .…”

Section: Introductionmentioning

confidence: 99%

A fluorescent probe for Hg 2+ specific recognition based on xanthene and its application in food detection and cell imaging

Zhang,

Nie,

Liu

et al. 2024

Preprint

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The mercury-loving unit aminothiourea was introduced into the xanthene fluorophore to synthesized the probe molecule NXH. NXH has a specific response to Hg2+, and with the addition of (0 ~ 50 µM) Hg2+, the fluorescence intensity of the probe solution was quenched from 2352 a.u. to about 308 a.u.. The probe NXH exhibited excellent detection performance of high sensitivity (LOD = 96.3 nM), real-time response (105 s), wide pH range (2.1 ~ 9.3), and strong anti-interference ability for Hg2+. At the same time, the probe NXH has wide range of applications for Hg2+ detection, which can be used to create molecular logic gates, make Hg2+ detection test paper, as well as the fluorescence imaging of Hg2+ in Hela live cells and tea samples.

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Section: Introductionmentioning

confidence: 99%

A Fluorescent Probe for Hg2+ Specific Recognition Based on Xanthene and its Application in Food Detection and Cell Imaging

Zhang,

Nie,

Liu

et al. 2024

J Fluoresc

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The mercury-loving unit aminothiourea was introduced into the xanthene uorophore to synthesized the probe molecule NXH. NXH has a speci c response to Hg 2+ , and with the addition of (0 ~ 50 µM) Hg 2+ , the uorescence intensity of the probe solution was quenched from 2352 a.u. to about 308 a.u.. The probe NXH exhibited excellent detection performance of high sensitivity (LOD = 96.3 nM), real-time response (105 s), wide pH range (2.1 ~ 9.3), and strong anti-interference ability for Hg 2+ . At the same time, the probe NXH has wide range of applications for Hg 2+ detection, which can be used to create molecular logic gates, make Hg 2+ detection test paper, as well as the uorescence imaging of Hg 2+ in Hela live cells and tea samples.

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Highly selective and sensitive detection of Hg2+ by a novel fluorescent probe with dual recognition sites

Cited by 14 publications

References 67 publications

Exploration of commercial cyclen-based chelators for mercury-197 m/g incorporation into theranostic radiopharmaceuticals

Exploration of commercial cyclen-based chelators for mercury-197 m/g incorporation into theranostic radiopharmaceuticals

A fluorescent probe for Hg 2+ specific recognition based on xanthene and its application in food detection and cell imaging

A Fluorescent Probe for Hg2+ Specific Recognition Based on Xanthene and its Application in Food Detection and Cell Imaging

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