| Ru(Ⅱ) Bipyridyl Complex and TiO2 Nanocomposite Based Biomolecule-free Photoelectrochemical Sensor for Highly Selective Determination of Ultra-trace Hg^2+ in Aqueous Systems |
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| 引用本文： | WU Shuo,YANG Xinlan,ZHAO Yanqiu. Ru(Ⅱ) Bipyridyl Complex and TiO2 Nanocomposite Based Biomolecule-free Photoelectrochemical Sensor for Highly Selective Determination of Ultra-trace Hg^2+ in Aqueous Systems[J]. 高等学校化学研究, 2019, 35(3): 370-376. DOI: 10.1007/s40242-019-8392-z |
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| 作者姓名： | WU Shuo YANG Xinlan ZHAO Yanqiu |
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| 作者单位： | School of Chemistry |
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| 基金项目： | the National Natural Science Foundation of China;the Foundamental Research Funds for the Central Universities of China;the Foundation of the State Key Laboratory of Analytical Chemistry for Life Science,China |
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| 摘 要： | A biomolecule-free photoelectrochemical(PEC) probe(denoted as Ru-1) was designed, synthesized and coupled with TiO2 nanoparticles(NPs) for the highly sensitive and selective PEC detection of Hg^2+, a model analyte with hypertoxicity to both human health and ecosystem. The probe Ru-1 was designed with Ru(Ⅱ) bipyridyl complex as the chromophore, thiocyanate ligand as the recognition unit, and carboxylate group as the linkage site to connect Ru-1 to TiO2 nanoparticles. Under irradiation, Ru-1 shows strong affinity to TiO2 and good photophysical properties of strong visible light absorption, slow electron-hole(e-h^+) recombination, and fast photoelectron injection to TiO2 nanoparticles via the bridge of 4-(2,2-bipyridin)-4-yl-thiophene moiety. However, the specific coordination of Hg^2+ with Ru-1 via the thiol moiety in the thiocyanate enlarges the band gap of tlie complex and reduces the photocurrent significantly. The synergistic interaction between TiO2 nanoparticles and the Ru-1 complex led to a selective PEC sensing strategy for Hg^2+ detection. Detectable linear ranges from 10^-12 g/mL to 10^-7 g/mL and from 10^-7g/mL to 10^-3 g/mL were obtained without the interference from possibly co-existed metal ions. The good analytical performances indicate the chemical probe based biomolecule-free PEC platform may offer a new route for the detection of biologically and environmentally important small molecules.
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| 关 键 词： | Photoelectrochemical probe Ru(II) BIPYRIDYL COMPLEX Hg2+ detection NANOCOMPOSITE |
| 收稿时间： | 2018-12-17 |
Ru(II) Bipyridyl Complex and TiO2 Nanocomposite Based Biomolecule-free Photoelectrochemical Sensor for Highly Selective Determination of Ultra-trace Hg2+ in Aqueous Systems |
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| WU Shuo,YANG Xinlan,ZHAO Yanqiu. Ru(II) Bipyridyl Complex and TiO2 Nanocomposite Based Biomolecule-free Photoelectrochemical Sensor for Highly Selective Determination of Ultra-trace Hg2+ in Aqueous Systems[J]. Chemical Research in Chinese University, 2019, 35(3): 370-376. DOI: 10.1007/s40242-019-8392-z |
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| Authors: | WU Shuo YANG Xinlan ZHAO Yanqiu |
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| Affiliation: | School of Chemistry, Dalian University of Technology, Dalian 116023, P. R. China |
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| Abstract: | A biomolecule-free photoelectrochemical(PEC) probe(denoted as Ru-1) was designed, synthesized and coupled with TiO2 nanoparticles(NPs) for the highly sensitive and selective PEC detection of Hg2+, a model analyte with hypertoxicity to both human health and ecosystem. The probe Ru-1 was designed with Ru(Ⅱ) bipyridyl complex as the chromophore, thiocyanate ligand as the recognition unit, and carboxylate group as the linkage site to connect Ru-1 to TiO2 nanoparticles. Under irradiation, Ru-1 shows strong affinity to TiO2 and good photophysical properties of strong visible light absorption, slow electron-hole(e-h+) recombination, and fast photoelectron injection to TiO2 nanoparticles via the π-bridge of 4-(2,2'-bipyridin)-4-yl-thiophene moiety. However, the specific coordination of Hg2+ with Ru-1 via the thiol moiety in the thiocyanate enlarges the band gap of the complex and reduces the photocurrent significantly. The synergistic interaction between TiO2 nanoparticles and the Ru-1 complex led to a selective PEC sensing strategy for Hg2+ detection. Detectable linear ranges from 10-12 g/mL to 10-7 g/mL and from 10-7 g/mL to 10-3 g/mL were obtained without the interference from possibly co-existed metal ions. The good analytical performances indicate the chemical probe based biomolecule-free PEC platform may offer a new route for the detection of biologically and environmentally important small molecules. |
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| Keywords: | Photoelectrochemical probe Ru(II) bipyridyl complex Hg2+ detection Nanocomposite |
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