<p>Fe<sup>III</sup>–Pr<sup>III</sup> Heterometallic Polyoxometalate Framework Applied as an Electrochemical Aptasensor for Dual-Mode Detection of Mucin 1</p>

<p>Achieving the high selectivity and sensitivity of biosensors for the early detection of diseases remains a major challenge. In this work, we have successfully fabricated a novel three-dimensional Fe<sup>III</sup>-Pr<sup>III</sup> heterometallic polyoxometalate framework (POMF) [Pr(H<sub>2</sub>O)<sub>4</sub>(pdc)]<sub>2</sub>Na<sub>2</sub>[Pr(H<sub>2</sub>O)<sub>7</sub>]<sub>2</sub>[Fe<sub>4</sub>(H<sub>2</sub>O)<sub>2</sub>(pdc)<sub>2</sub>(B-<em>β</em>-SbW<sub>9</sub>O<sub>33</sub>)<sub>2</sub>]∙16H<sub>2</sub>O (1, H<sub>2</sub>pdc = pyridine-2,5-dicarboxylic acid). Notably, the tetra-Fe<sup>3+</sup>-substituted [Fe<sub>4</sub>(H<sub>2</sub>O)<sub>2</sub>(pdc)<sub>2</sub>(B -<em>β</em>-SbW<sub>9</sub>O<sub>33</sub>)<sub>2</sub>]<sup>10-</sup> unit can be considered as derived from electrochemically active Krebs-type [Fe<sub>4</sub>(H<sub>2</sub>O)<sub>10</sub>(B-<em>β</em>-SbW<sub>9</sub>O<sub>33</sub>)<sub>2</sub>]<sup>6- </sup>unit through the replacement of highly reactive aqua ligands with H<sub>2</sub>pdc. Subsequently, [Fe<sub>4</sub>(H<sub>2</sub>O)<sub>2</sub>(pdc)<sub>2</sub>(B-<em>β</em>-SbW<sub>9</sub>O<sub>33</sub>)<sub>2</sub>]<sup>10-</sup> units coordinate with Pr<sup>3+</sup> cations to form the Fe<sup>III</sup>-Pr<sup>III</sup> heterometallic POMF. Furthermore, this heterometallic POMF was employed to construct an electrochemical aptasensor capable of sensitive detection of mucin 1, a tumor biomarker. This aptasensor enables dual-mode detection of mucin 1 with low detection limits of 0.126 pg· mL<sup>-1</sup> and 0.129 pg· mL<sup>-1</sup>, as determined by electrochemical impedance spectroscopy and differential pulse voltammetry, respectively. This work not only presents a viable strategy for constructing advanced heterometallic POMFs, but also establishes a new electrochemical biosensing platform for detecting tumor marker proteins.</p>

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Publication Details

Published
2025-09-23
DOI
https://doi.org/10.20517/scierxiv202509.0630.v1
Primary Topic
Polyoxometalates: Synthesis and Applications
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article
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article

<p>FeIII–PrIII Heterometallic Polyoxometalate Framework Applied as an Electrochemical Aptasensor for Dual-Mode Detection of Mucin 1</p>

Zhigang Tang, Jiaxin Li, Lijuan Chen, Junwei Zhao
Polyoxometalates: Synthesis and Applications
article

<p>FeIII–PrIII Heterometallic Polyoxometalate Framework Applied as an Electrochemical Aptasensor for Dual-Mode Detection of Mucin 1</p>

Zhigang Tang, Jiaxin Li, Lijuan Chen, Junwei Zhao
article en

Abstract

&lt;p&gt;Achieving the high selectivity and sensitivity of biosensors for the early detection of diseases remains a major challenge. In this work, we have successfully fabricated&amp;nbsp;a novel three-dimensional Fe&lt;sup&gt;III&lt;/sup&gt;-Pr&lt;sup&gt;III&lt;/sup&gt;&amp;nbsp;heterometallic polyoxometalate framework&amp;nbsp;(POMF)&amp;nbsp;[Pr(H&lt;sub&gt;2&lt;/sub&gt;O)&lt;sub&gt;4&lt;/sub&gt;(pdc)]&lt;sub&gt;2&lt;/sub&gt;Na&lt;sub&gt;2&lt;/sub&gt;[Pr(H&lt;sub&gt;2&lt;/sub&gt;O)&lt;sub&gt;7&lt;/sub&gt;]&lt;sub&gt;2&lt;/sub&gt;[Fe&lt;sub&gt;4&lt;/sub&gt;(H&lt;sub&gt;2&lt;/sub&gt;O)&lt;sub&gt;2&lt;/sub&gt;(pdc)&lt;sub&gt;2&lt;/sub&gt;(B-&lt;em&gt;β&lt;/em&gt;-SbW&lt;sub&gt;9&lt;/sub&gt;O&lt;sub&gt;33&lt;/sub&gt;)&lt;sub&gt;2&lt;/sub&gt;]∙16H&lt;sub&gt;2&lt;/sub&gt;O&amp;nbsp;(1, H&lt;sub&gt;2&lt;/sub&gt;pdc = pyridine-2,5-dicarboxylic acid). Notably, the tetra-Fe&lt;sup&gt;3+&lt;/sup&gt;-substituted [Fe&lt;sub&gt;4&lt;/sub&gt;(H&lt;sub&gt;2&lt;/sub&gt;O)&lt;sub&gt;2&lt;/sub&gt;(pdc)&lt;sub&gt;2&lt;/sub&gt;(B&amp;nbsp;-&lt;em&gt;β&lt;/em&gt;-SbW&lt;sub&gt;9&lt;/sub&gt;O&lt;sub&gt;33&lt;/sub&gt;)&lt;sub&gt;2&lt;/sub&gt;]&lt;sup&gt;10-&lt;/sup&gt;&amp;nbsp;unit can be considered as&amp;nbsp;derived from electrochemically active Krebs-type [Fe&lt;sub&gt;4&lt;/sub&gt;(H&lt;sub&gt;2&lt;/sub&gt;O)&lt;sub&gt;10&lt;/sub&gt;(B-&lt;em&gt;β&lt;/em&gt;-SbW&lt;sub&gt;9&lt;/sub&gt;O&lt;sub&gt;33&lt;/sub&gt;)&lt;sub&gt;2&lt;/sub&gt;]&lt;sup&gt;6-&amp;nbsp;&lt;/sup&gt;unit&amp;nbsp;through the replacement of highly reactive aqua ligands with H&lt;sub&gt;2&lt;/sub&gt;pdc. Subsequently, [Fe&lt;sub&gt;4&lt;/sub&gt;(H&lt;sub&gt;2&lt;/sub&gt;O)&lt;sub&gt;2&lt;/sub&gt;(pdc)&lt;sub&gt;2&lt;/sub&gt;(B-&lt;em&gt;β&lt;/em&gt;-SbW&lt;sub&gt;9&lt;/sub&gt;O&lt;sub&gt;33&lt;/sub&gt;)&lt;sub&gt;2&lt;/sub&gt;]&lt;sup&gt;10-&lt;/sup&gt;&amp;nbsp;units coordinate with Pr&lt;sup&gt;3+&lt;/sup&gt;&amp;nbsp;cations to form the Fe&lt;sup&gt;III&lt;/sup&gt;-Pr&lt;sup&gt;III&lt;/sup&gt;&amp;nbsp;heterometallic POMF. Furthermore, this heterometallic POMF was employed to construct&amp;nbsp;an electrochemical aptasensor capable of sensitive detection of mucin 1, a tumor biomarker. This aptasensor&amp;nbsp;enables dual-mode detection of mucin 1 with low detection limits of 0.126 pg·&amp;nbsp;mL&lt;sup&gt;-1&lt;/sup&gt;&amp;nbsp;and 0.129 pg·&amp;nbsp;mL&lt;sup&gt;-1&lt;/sup&gt;, as determined by electrochemical impedance spectroscopy&amp;nbsp;and differential pulse voltammetry, respectively.&amp;nbsp;This work not only presents a viable strategy for constructing advanced&amp;nbsp;heterometallic POMFs, but also establishes a new electrochemical biosensing platform for detecting tumor marker proteins.&lt;/p&gt;

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