title: Simple and rapid mercury ion selective electrode based on 1-undecanethiol assembled Au substrate and its recognition mechanism.
abstract: A simple and rapid mercury ion selective electrode based on 1-undecanethiol (1-UDT) assembled Au substrate (Au/1-UDT) has been well constructed. 1-UDT was for the purpose of generating self-assembled monolayer on gold surface to recognize Hg2+in aqueous solution, which had a working concentration range of 1.0×10-8-1.0×10-4molL-1, with a Nernst response slope of 28.83±0.4mV/-pC, a detection limit of 4.5×10-9molL-1, and a good selectivity over the other tested cations. Also, the Au/1-UDT possessed good reproducibility, stability, and short response time. The recovery obtained for the determination of mercury ion in practical tremella samples was in the range of 99.8-103.4%. Combined electrochemical analysis and X-ray photoelectron spectroscopy (XPS) with quantum chemical computation, the probable recognition mechanism of the electrode for selective recognition of Hg2+has been investigated. The covalent bond formed between mercury and sulfur is stronger than the one between gold and sulfur and thus prevents the adsorption of 1-UDT molecules on the gold surface. The quantum chemical computation with density functional theory further demonstrates that the strong interaction between the mercury atom and the sulfur atom on the gold surface leads to the gold sulfur bond ruptured and the gold mercury metallophilic interaction.
authors.affiliation: Hunan Provincial Key Laboratory of Materials Protection for Electric Power and Transportation, School of Chemistry and Biological Engineering, Changsha University of Science and Technology, Changsha 410114, PR China.
authors.forename: Xian-Qing
authors.initials: XQ
authors.lastname: Li
authors.affiliation: Hunan Provincial Key Laboratory of Materials Protection for Electric Power and Transportation, School of Chemistry and Biological Engineering, Changsha University of Science and Technology, Changsha 410114, PR China.
authors.forename: Hai-Qing
authors.initials: HQ
authors.lastname: Liang
authors.affiliation: Hunan Provincial Key Laboratory of Materials Protection for Electric Power and Transportation, School of Chemistry and Biological Engineering, Changsha University of Science and Technology, Changsha 410114, PR China. Electronic address: zhongcao2004@163.com.
authors.forename: Zhong
authors.initials: Z
authors.lastname: Cao
authors.affiliation: Hunan Provincial Key Laboratory of Materials Protection for Electric Power and Transportation, School of Chemistry and Biological Engineering, Changsha University of Science and Technology, Changsha 410114, PR China.
authors.forename: Qing
authors.initials: Q
authors.lastname: Xiao
authors.affiliation: Hunan Provincial Key Laboratory of Materials Protection for Electric Power and Transportation, School of Chemistry and Biological Engineering, Changsha University of Science and Technology, Changsha 410114, PR China; State Key Laboratory of High Performance Complex Manufacturing, School of Mechanical and Electrical Engineering, Central South University, Changsha 410083, PR China. Electronic address: xiaozhongliang@163.com.
authors.forename: Zhong-Liang
authors.initials: ZL
authors.lastname: Xiao
authors.affiliation: Hunan Provincial Key Laboratory of Materials Protection for Electric Power and Transportation, School of Chemistry and Biological Engineering, Changsha University of Science and Technology, Changsha 410114, PR China.
authors.forename: Liu-Bin
authors.initials: LB
authors.lastname: Song
authors.affiliation: Hunan Airbluer Environmental Protection Technology Co., Ltd., Changsha 410014, PR China.
authors.forename: Dan
authors.initials: D
authors.lastname: Chen
authors.affiliation: State Key Laboratory of High Performance Complex Manufacturing, School of Mechanical and Electrical Engineering, Central South University, Changsha 410083, PR China.
authors.forename: Fu-Liang
authors.initials: FL
authors.lastname: Wang
mesh_terms: D058266:Dielectric Spectroscopy; D055664:Electrochemical Techniques; D006046:Gold / Q000737:chemistry*; D006863:Hydrogen-Ion Concentration; D017736:Ion-Selective Electrodes; D007477:Ions / Q000737:chemistry; D057230:Limit of Detection; D008628:Mercury / Q000032:analysis*; D008855:Microscopy, Electron, Scanning; D056951:Photoelectron Spectroscopy; D011789:Quantum Theory; D015203:Reproducibility of Results; D013438:Sulfhydryl Compounds / Q000737:chemistry*; D013499:Surface Properties
chemical_list: D007477:Ions; D013438:Sulfhydryl Compounds; D006046:Gold; D008628:Mercury; C000617854:1-undecanethiol
keywords: 1-Undecanethiol; Density functional theory; Mercury ion; Recognition mechanism; Self-assembled monolayer