Ytterbium-incorporated porphyrin nanostructure-modified carbon electrodes for ultra-sensitive detection of lead ions in water environments

IF 9.5 2区 材料科学 Q1 CHEMISTRY, PHYSICAL
Zeyu Liu, Yao Liu, Qiang Xue, Lin He, Hao Liu, Jianwei Zhao
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Abstract

Simple modification of electrodes for sensitive Pb(II) detection is the key to the realization of electrochemical sensors for monitoring water pollution, but it remains a challenge. In this study, a novel ytterbium (Yb)-functionalized meso-tetra(4-carboxyphenyl)porphyrin (Yb-TCPP) composite was synthesized via a hydrothermal method to address this challenge. The excellent structure and properties of Yb-TCPP significantly enhance the sensitivity (783.58 μA μM−1 cm−2) of electrochemical Pb(II) detection by the electrode. The Yb-TCPP-modified electrode exhibits a strong linear relationship in the Pb(II) concentration ranges of 5–300 μg L−1 and 300–1000 μg L−1, with a detection limit as low as 0.16 μg L−1. The recovery rate obtained from repeated testing of actual water samples ranged from 98.93% to 100.63%. Density functional theory (DFT) was used to predict the structure of Yb-TCPP, which confirms that a large number of tetrapyrrolic cavities with strong adsorption to Pb are retained in the structure. The decrease in the structural energy gap further proves that Yb improves the conductivity of the material. The electron transfer in the system is revealed, and Yb-TCPP shows strong catalytic effects in both the reduction-enrichment and oxidation-stripping stages of Pb. This study discards the previous redundant modification process of multi-material composites and provides a new idea for the modification of a single-material electrode, which advances practical applications in environmental heavy metal monitoring.

Abstract Image

含镱卟啉纳米结构修饰碳电极用于水环境中铅离子的超灵敏检测
对电极进行简单修饰以实现对Pb(II)的灵敏检测是实现电化学传感器监测水污染的关键,但这仍然是一个挑战。在本研究中,通过水热法合成了一种新型的镱(Yb)功能化中四(4-羧基苯基)卟啉(Yb- tcpp)复合物来解决这一挑战。Yb-TCPP优良的结构和性能显著提高了电极电化学检测Pb(II)的灵敏度(783.58 μA μM−1 cm−2)。yb - tpcp修饰电极在Pb(II)浓度5 ~ 300 μg L−1和300 ~ 1000 μg L−1范围内呈良好的线性关系,检出限低至0.16 μg L−1。实际水样重复检测的回收率为98.93% ~ 100.63%。利用密度泛函理论(DFT)对Yb-TCPP的结构进行了预测,证实其结构中保留了大量对Pb具有强吸附作用的四吡咯腔。结构能隙的减小进一步证明Yb提高了材料的导电性。结果表明,Yb-TCPP在Pb的还原-富集和氧化-溶出两个阶段均表现出较强的催化作用。该研究摒弃了以往多材料复合材料的冗余改性工艺,为单材料电极的改性提供了新的思路,推进了环境重金属监测的实际应用。
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来源期刊
Journal of Materials Chemistry A
Journal of Materials Chemistry A CHEMISTRY, PHYSICAL-ENERGY & FUELS
CiteScore
19.50
自引率
5.00%
发文量
1892
审稿时长
1.5 months
期刊介绍: The Journal of Materials Chemistry A, B & C covers a wide range of high-quality studies in the field of materials chemistry, with each section focusing on specific applications of the materials studied. Journal of Materials Chemistry A emphasizes applications in energy and sustainability, including topics such as artificial photosynthesis, batteries, and fuel cells. Journal of Materials Chemistry B focuses on applications in biology and medicine, while Journal of Materials Chemistry C covers applications in optical, magnetic, and electronic devices. Example topic areas within the scope of Journal of Materials Chemistry A include catalysis, green/sustainable materials, sensors, and water treatment, among others.
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