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Colorimetric determination of As(III) based on 3-mercaptopropionic acid assisted active site and interlayer channel dual-masking of Fe-Co-layered double hydroxides with oxidase-like activity

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Abstract

A colorimetric method is described for the determination of As(III). It is based on the use of 3-mercaptopropionic acid (3-MPA) assisted active site and interlayer channel dual-masking of oxidase-like Fe-Co-layered double hydroxides (Fe-Co-LDH). The Fe-Co-LDH acts as an oxidase-mimicking nanozyme with high activity. It catalyzes the oxidation of colorless 3,3′5,5′-tetramethylbenzidine (TMB) to form a blue product (oxTMB) with an absorption maximum at 652 nm. It is found that As(III) firmly anchors onto the Fe* sites of the 3-MPA-modified Fe-Co-LDH via forming a stable Fe─As(III)─3-MPA─As(III)─Fe structure. This results in masking the active sites and interlayer channels of the Fe-Co-LDH nanozyme. As a result, the presence of As(III) as well as 3-MPA specifically inhibit the LDH-catalyzed chromogenic reaction. Based on the above principle, a colorimetric assay was designed for the determination of As(III). It provided linear response in the 0.10~8.33 μM As(III) concentration range and a detection limit as low as 35 nM. The assay was applied to the quantitation of As(III), even in the presence of potential interferents including As(V), Hg(II) and Pb(II), in environmental and drinking water samples.

Schematic illustration of the As(III) sensing mechanism based on 3-mercaptopropionic acid (3-MPA) assisted active site and interlayer channel dual-masking of Fe-Co-layered double hydroxides (Fe-Co-LDH) with oxidase-like activity. 3-MPA with sulfhydryl and carboxyl groups can assist As(III) to firmly anchor onto the Fe* sites inside the interlayer channels of the Fe-Co-LDH via forming a Fe─As(III)─3-MPA─As(III)─Fe structure, thus selectively resulting in a significant suppression of the chromogenic reaction.

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Acknowledgements

This work is financially supported by the National Natural Science Foundation of China (21605061), the Natural Science Foundation of Jiangsu Province (BK20160489), the Cultivation Project for Excellent Young Teachers of Jiangsu University, and the Postgraduate Research & Practice Innovation Program of Jiangsu Province (No. KYCX18_2275).

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Authors and Affiliations

  1. School of Food and Biological Engineering, Jiangsu University, Zhenjiang, 212013, China

    Xuechao Xu, Xiaobo Zou & Shuwen Wu

  2. Institute of Green Chemistry and Chemical Technology, School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang, 212013, China

    Xuechao Xu, Linjie Wang, Jianming Pan, Minjin Xu, Wen Shan, Xin Li & Xiangheng Niu

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  1. Xuechao Xu
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  2. Xiaobo Zou
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Correspondence to Xiaobo Zou, Jianming Pan or Xiangheng Niu.

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Xu, X., Zou, X., Wu, S. et al. Colorimetric determination of As(III) based on 3-mercaptopropionic acid assisted active site and interlayer channel dual-masking of Fe-Co-layered double hydroxides with oxidase-like activity. Microchim Acta 186, 815 (2019). https://doi.org/10.1007/s00604-019-3835-5

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