Smart Two-dimensional Photonic Crystal Hydrogel for Accurate Detection of Hg2+

doi:10.6023/A23100443

Abstract

A smart two-dimensional photonic crystal (2DPC) hydrogel was developed for accurate detection of Hg²⁺ by combining the Debye diffraction effect of 2DPC and the volume phase transition characteristic of hydrogel. The polystyrene (PS) 2DPC arrays were first fabricated by needle-tip-flow method, in which the monodispersed PS microspheres were orderly self-assembled on the water surface to form PS 2DPC and then transferred to glass slide. The poly(acrylamide-allylthiourea) hydrogels embedded with the PS 2DPC arrays were fabricated by “sandwich” method, in which the polymerization precursor solution including monomers acrylamide and allylthiourea was added to the PS 2DPC surface and covered with a glass slide, followed by photopolymerization. The atoms including N, O and S from functional groups on the hydrogel chains selectively coordinated with Hg²⁺, shortening the distance between the hydrogel chains and increasing the crosslinking density of the hydrogel. As a result, the hydrogel shrank and the PS microsphere spacing of the 2DPC decreased, which increased the diameter of the Debye diffraction ring. The microsphere spacing changes were acquired by monitoring Debye diffraction ring diameters before and after the response of the 2DPC hydrogel, achieving the highly sensitive, selective, reversible and fast detection of Hg²⁺. The linear detection ranges were in 10~100 nmol/L and 25~200 μmol/L, and the limit of detection was found to be 3.32 nmol/L. The prepared smart 2DPC hydrogel was used to detect Hg²⁺ in cosmetics and water samples to evaluate its practicability. The recovery for the detection of Hg²⁺ was 98.8%~102.6% and the relative standard deviation was 0.57%~1.09% for a commercially lipstick, and they were 97.2%~103.4% and 0.61%~0.99% for the tap water, respectively. The results demonstrated that our constructed smart 2DPC hydrogels have good applicability, accuracy and reliability for the detection of Hg²⁺ in real samples. The method is simple for testing, only requiring a laser pointer and a ruler, without needing sophisticated instruments, and it can realize portable detection, providing a new strategy for detecting metal ions.

Key words: two-dimensional photonic crystals, Debye diffraction effect, smart hydrogel, volume phase transition, mercury ions

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Yuqing Shi, Mingzhu Chu, Bo Han, Haojie Ma, Ran Li, Xueyan Hou, Yuqi Zhang, Ji-Jiang Wang. Smart Two-dimensional Photonic Crystal Hydrogel for Accurate Detection of Hg²⁺[J]. Acta Chimica Sinica, 2024, 82(1): 9-15.

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Fig. & Tab. 6

Figure 1. SEM images: (a, b) PS 2DPC on glass slide; (c) the freshly prepared P(AAm-ATU)-PS 2DPCH; (d) the P(AAm-ATU)-PS 2DPCH after equilibration in PBS solution. Insets: the photographs of the corresponding films

Figure 2. The particle spacing changes of P(AAm-ATU)-PS 2DPCH and PAAm-PS 2DPCH after reaction with various solutions

Figure 3. (a) The polymerization reaction of P(AAm-ATU) hydrogel and the interaction with Hg2+. Hydrogels were prepared by photoinitiated polymerization using AAm and ATU as monomers and BIS as crosslinker. The atoms including N, O, and S on the chains of the hydrogel coordinate with Hg2+, leading to volume shrinkage of the hydrogel. The coordinated Hg2+ can be eluted by HCl aqueous solution to regenerate the sensing film. (b) The schematic illustration for interaction of P(AAm-ATU)-PS 2DPCH and Hg2+, and the photographs of the corresponding Debye diffraction rings. The d represents the microsphere spacing and D represents the diameter of the Debye diffraction ring. The hydrogel shrinks after reaction with Hg2+, resulting in a decrease in microsphere spacing of the embedded PS 2DPC array (from d to d'). The corresponding Debye diffraction ring diameter increases from D to D'

Figure 4. After response to Hg2+ at different concentrations, the microsphere spacing changes of the various P(AAm-ATU)-PS 2DPCH fabricated from (a) BIS at different concentrations and (b) different mass ratio of AAm/ATU

Figure 5. (a) Dependence of microsphere spacing change of P(AAm-ATU)-PS 2DPCH on the concentration of Hg2+; (b, c) linear relationship between microsphere spacing change and the concentration of Hg2+; (d) microsphere spacing changes for the P(AAm-ATU)-PS 2DPCH in various metal ions solutions (200 μmol/L). Inset: the photographs of P(AAm-ATU)-PS 2DPCH before and after response to Hg2+; (e) time dependence of microsphere spacing changes for the P(AAm-ATU)-PS 2DPCH in Hg2+ at different concentrations; (f) the particle spacing of P(AAm-ATU)-PS 2DPCH after alternate reaction to Hg2+ (200 μmol/L) and HCl (1 mol/L)

Sample	Added	Found	Recovery/%	RSD/% (n=3)
口红	50 nmol/L	50.2 nmol/L	100.4	0.76
	50 µmol/L	51.3 μmol/L	102.6	1.09
	100 µmol/L	98.8 μmol/L	98.8	0.57
自来水	50 nmol/L	50.2 nmol/L	100.4	0.61
	50 µmol/L	51.7 μmol/L	103.4	0.99
	100 µmol/L	97.2 μmol/L	97.2	0.86

Table 1. The detection of Hg2+ in real samples

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智能二维光子晶体水凝胶精准检测Hg²⁺

Smart Two-dimensional Photonic Crystal Hydrogel for Accurate Detection of Hg²⁺

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智能二维光子晶体水凝胶精准检测Hg2+