基于PbS QDs/TiO2 NPs构建新型谷胱甘肽光电化学传感器

doi:10.7503/cjcu20190106

摘要/Abstract

摘要：

通过高温煅烧将二氧化钛纳米颗粒(TiO₂ NPs)修饰到ITO电极表面制成TiO₂ NPs/ITO电极, 再采用连续离子层吸附反应(SILAR)循环将硫化铅量子点(PbS QDs)修饰到TiO₂/ITO电极表面制得PbS QDs/TiO₂ NPs/ITO电极, 并将该电极应用于检测谷胱甘肽(GSH)的光电化学传感器. 在该传感器中, 当PbS QDs受470 nm可见光的激发时将产生电子(e)和光生空穴(h ⁺), 光生空穴可被溶液中的GSH捕获, 并将GSH氧化成GSSH, 有效避免电子和空穴的复合, 显著提高了光电效率. 该传感器对GSH的检测具有较高的灵敏度和选择性, 线性检测范围为0.06~1 mmol/L, 检出限(LOD)为4.6×10 ^-3 mmol/L(S/N=3).

关键词: 硫化铅量子点, 二氧化钛纳米颗粒, 谷胱甘肽, 光电化学, 生物传感器

Abstract:

Firstly, titanium dioxide nanoparticles(TiO₂ NPs) was modified to the surface of indium tin oxide(ITO) electrode by high-temperature calcination to prepare TiO₂ NPs/ITO electrode. And then sulfide quantum dots(PbS QDs) were modified to the surface of TiO₂ NPs/ITO electrode by successive ionic layer adsorption and reaction(SILAR) cycle to prepare the PbS QDs/TiO₂ NPs/ITO electrode. And it was used to detect glutathione(GSH). In this sensor, when PbS QDs are excited by 470 nm visible light, it will produce electrons(e) and holes(h ⁺). Immediately after, h ⁺ will be captured by GSH in solution, and then GSH is oxidized into GSSH. Therefore, the recombination of electrons and holes were avoided effectively. Thus the photoelectric efficiency has been significantly improved. This sensor had satisfactory sensitivity and selectivity for GSH. what’s more, the detection range is 0.06—1 mmol/L, and the detection limit(LOD) is 4.6×10 ^-3 mmol/L(S/N=3).

Key words: PbS QDs, TiO₂ NPs, Glutathione(GSH), Photoelectrochemical, Biosensor

中图分类号:

O652.1

郑姗, 刘洋, 陈飘飘, 邢怡晨, 黄朝表. 基于PbS QDs/TiO₂ NPs构建新型谷胱甘肽光电化学传感器[J]. 高等学校化学学报, 2019, 40(9): 1866-1872.

ZHENG Shan, LIU Yang, CHEN Piaopiao, XING Yichen, HUANG Chaobiao. Novel Glutathione Photoelectrochemical Sensor Based on PbS QDs/TiO₂ NPs ^†[J]. Chemical Journal of Chinese Universities, 2019, 40(9): 1866-1872.

图/表 13

Fig.1 SEM images of TiO2 NPs/ITO(A) and PbS QDs/TiO2 NPs/ITO(B) electrodes

Fig.2 XRD patterns of ITO(a), TiO2 NPs/ITO(b) and PbS QDs/TiO2 NPs/ITO(c) electrodes

Fig.3 Full-scan XPS spectra of TiO2 NPs and PbS QDs/TiO2 NPs electrodes(A) and high-resolution XPS spectra of Ti2p(B), O1s(C), Pb4f(D) and S2p(E) of PbS QDs/TiO2 NPs electrode

Fig.4 EIS of TiO2 NPs/ITO(a) and PbS QDs/TiO2 NPs/ITO(b) electrodes The EIS measurements are carried out in 0.1 mol/L KCl containing 5.0 mmol/L K3Fe(CN)6/K4Fe(CN)6(1∶1), The frequency range was between 0.1 and 1×105 Hz with an applied voltage of 5 mV. Inset: equivalent circuit diagram. Cd: capacitance; Rct: charge transfer resistance; Ru: ohmic resistance; Zw: diffusion resistance.

Fig.5 Effect of TiO2 NPs concentration on photocurrent responses of the sensor

Fig.6 Effect of SILAR cycle times on photocurrent responses of the sensor

Fig.7 Effect of wavelength on photocurrent responses of the sensor

Fig.8 Effect of potential on photocurrent responses of the sensor

Fig.9 Photocurrent response curves of different modified ITO(a), TiO2/ITO(b), PbS QDs/TiO2/ITO(c) and QDs/TiO2/ITO(d) electrodes in 0.2 mmol/L GSH/PbS

Fig.10 Preparation process diagram(A) and mechanism diagram(B) of GSH sensor

Fig.11 Linear calibration curve GSH sensor Inset: Photocurrent response of GSH sensor.

Fig.12 Stability of PbS QDs/TiO2 NPs/ITO electrode

Fig.13 Photocurrent signals of the GSH sensor toward in the presence of 1 mmol/L cysteine(Cys), alanine(Ala), dopamine(DA), glycine(Gly), leucine(Lue), arginine(Arg), valine(Val), glucose(Glu) and all their mixture(Mix) and 0.2 mmol/L GSH

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基于PbS QDs/TiO₂ NPs构建新型谷胱甘肽光电化学传感器

Novel Glutathione Photoelectrochemical Sensor Based on PbS QDs/TiO₂ NPs ^†

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