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<p>Arsenic (As), particularly in its bioavailable species of inorganic As(Ⅲ) known for its significant toxicity and mobility, is a carcinogenic risk to humans. Serving as an innovative analytical tool, the diffusive gradients in thin films (DGT) technique facilitates on-site detection of bioavailable metals. However, the options of DGT binding gels tailored for As(Ⅲ) detection remain elusive. This study undertook the modification of tetraethyl orthosilicate with a 3-mercaptopropyl-trimethoxysilane to synthesize cost-effective nanomaterials endowed with the capacity for selective adsorption of As(Ⅲ) through copolymerization and atmospheric pressure drying. The synthesized materials were systematically characterized using X-ray diffraction, scanning electron microscopy, and C/H/N/S elemental analysis, revealing a specific surface area of 472.39&#xa0;m<sup>2</sup>/g, a particle size of 12.7&#xa0;nm, and a loading capacity of 3.115&#xa0;mmol/g. The DGT combined with gel prepared from this material has a specific affinity for As(III) without adsorbing As(V).Its adsorption efficiency for As(III) may reach 84.5% within the first hour. This DGT technique has a linear detection range of 0.5–15&#xa0;mg/L (R<sup>2</sup> = 0.99995), an elution recovery of 85.1%–102.7% (RSD &lt; 10%, n = 3), and a maximum adsorption capacity of 301.7&#xa0;μg/cm<sup>2</sup>, meeting requirements for long-term environmental monitoring. The experiment studied the effects of interfering factors, including pH values ranging from 3–9, ionic strength of 10–500&#xa0;mmol/L NaNO₃, Fe<sup>2</sup>⁺ 0–5.0&#xa0;mg/L, Mn<sup>2</sup>⁺ 0–1.0&#xa0;mg/L, As(V) 0–5.0&#xa0;mg/L, dissolved organic carbon 0–20.0&#xa0;mg/L, SO₄<sup>2</sup>⁻ 0.55–1.10&#xa0;g/L, and PO₄<sup>3</sup>⁻ 5.0–10.0&#xa0;mg/L. The device maintained a stable treatment performance under all these conditions. When the DGT device was deployed in spiked river water, estuarine water, and seawater, a comparison of its adsorption performance with existing methods showed that the device had a comparable adsorption performance and demonstrated excellent long-term stability in practical water environment applications.</p>

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Development and validation of a copolymerized thiol-silica based DGT technique for the assessment of bioavailable As(Ⅲ) speciation

  • 期刊论文

  • 发表日期：

    2026年3月10日

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  • Yue Zeng,
  • Zhennan Liu,
  • Yajie Jiang,
  • Yunqin Li,
  • Wei Yu,
  • Rong Yu,
  • Xiang Xu,
  • Meiling Xiao

摘要

Arsenic (As), particularly in its bioavailable species of inorganic As(Ⅲ) known for its significant toxicity and mobility, is a carcinogenic risk to humans. Serving as an innovative analytical tool, the diffusive gradients in thin films (DGT) technique facilitates on-site detection of bioavailable metals. However, the options of DGT binding gels tailored for As(Ⅲ) detection remain elusive. This study undertook the modification of tetraethyl orthosilicate with a 3-mercaptopropyl-trimethoxysilane to synthesize cost-effective nanomaterials endowed with the capacity for selective adsorption of As(Ⅲ) through copolymerization and atmospheric pressure drying. The synthesized materials were systematically characterized using X-ray diffraction, scanning electron microscopy, and C/H/N/S elemental analysis, revealing a specific surface area of 472.39 m2/g, a particle size of 12.7 nm, and a loading capacity of 3.115 mmol/g. The DGT combined with gel prepared from this material has a specific affinity for As(III) without adsorbing As(V).Its adsorption efficiency for As(III) may reach 84.5% within the first hour. This DGT technique has a linear detection range of 0.5–15 mg/L (R2 = 0.99995), an elution recovery of 85.1%–102.7% (RSD < 10%, n = 3), and a maximum adsorption capacity of 301.7 μg/cm2, meeting requirements for long-term environmental monitoring. The experiment studied the effects of interfering factors, including pH values ranging from 3–9, ionic strength of 10–500 mmol/L NaNO₃, Fe2⁺ 0–5.0 mg/L, Mn2⁺ 0–1.0 mg/L, As(V) 0–5.0 mg/L, dissolved organic carbon 0–20.0 mg/L, SO₄2⁻ 0.55–1.10 g/L, and PO₄3⁻ 5.0–10.0 mg/L. The device maintained a stable treatment performance under all these conditions. When the DGT device was deployed in spiked river water, estuarine water, and seawater, a comparison of its adsorption performance with existing methods showed that the device had a comparable adsorption performance and demonstrated excellent long-term stability in practical water environment applications.