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Selective coordination and localized polarization in graphene quantum dots: Detection of fluoride anions using ultra-low-field NMR relaxometry

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Chinese Chemical Letters 2021年第12期32卷 3921-3926页

作者： Yongqiang Li Yi Xiao Quan Tao Mengmeng Yu Li Zheng Siwei Yang Guqiao Ding Hui Dong Xiaoming Xie State Key Laboratory of Functional Materials of Informatics Shanghai Institute of Microsystem and Information TechnologyChinese Academy of Sciences(CAS)Shanghai 200050China CAS Center for Excellence in Superconducting Electronics(CENSE) Chinese Academy of SciencesShanghai 200050China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China

The development of ultra-sensitive methods for detecting anions is limited by their low charge to radius ratios, microenvironment sensitivity, and p H sensitivity. In this paper, a magnetic sensor is devised that exploits the controllable and selective coordination that occurs between a magnetic graphene quantum dot(GQD) and fluoride anion(F–). The sensor is used to measure the change in relaxation time of aqueous solutions of magnetic GQDs in the presence of F–using ultra-low-field(118 μT) nuclear magnetic resonance relaxometry. The method was optimized to produce a limit of detection of 10 nmol/L and then applied to quantitatively detect F–in domestic water samples. More importantly, the key factors responsible for the change in relaxation time of the magnetic GQDs in the presence of F–are revealed to be the selective coordination that occurs between the GQDs and F–as well as the localized polarization of the water protons. This striking finding is not only significant for the development of other magnetic probes for sensing anions but also has important ramifications for the design of contrast agents with enhanced relaxivity for use in magnetic resonance imaging.

关键词： Graphene quantum dots Coordination Polarization Relaxometry Magnetic sensor Nuclear magnetic resonance fluoride anion

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A Benzodithiophene-Based Fluorescence Probe for Rapid Detection of fluoride Ion

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Chinese Journal of Chemistry 2016年第8期34卷 809-813页

作者： Wenbin Tan Taohua Leng Guoqiao Lai Zhifang Li JiefeiWu Yongjia Shen Chengyun Wang Key Laboratory for Advanced Materials and Institute of Fine Chemicals East China University of Science and Technology Shanghai 200237 China National Food Quality Supervision and Inspection Center (Shanghai)/Shanghai Institute of Quality Inspection and Technical Research Shanghai 200233 China Key Laboratory of Organosilicon Chemistry and Material Technology of Ministry of Education Hangzhou Nor- mal University Hangzhou Zhejiang 310012 China

A novel and simple fluorescence probe was synthesized from benzo[1,2‐ b :4,5‐ b ′]dithiophene (BDT) and trimethylsilylethyne via Sonogashira reaction, and showed highly selective and sensitive fluorescence decreasing response towards F − . The probe molecule turned to a weakly fluorescent terminal alkyne moiety because its trimethylsilyl (TMS) group was cleaved by fluoride, which was proved by 1 H NMR titration. Whereas no distinct fluorescent changes were observed with the addition of other anions, such as Cl − , Br − , I − , AcO − and H 2 PO 4 − . Upon the addition of F − , the maximum fluorescence emission wavelength shifted from 460 nm to 450 nm with a decrease of fluorescence intensity by 40% within 20 s. Moreover, the detection limit towards F − was calculated to be as low as 73.5 nmol/L.

关键词： fluorescent probe benzodithiophene fluoride anion trimethylsilylethynyl group

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Reversible Disassembly and Intercalation of 2-Ureido-4[1 H]- Pyrimidinone Quadruple Hydrogen-bonded Supramolecular Assembly by fluoride and Lead Ions

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Chinese Journal of Chemistry 2011年第12期29卷 2684-2688页

作者：俞茂林赵春常冯科陈彬佟振合吴骊珠 Key Laboratory of Photochemical Conversion and Optoelectronic Materials Technical Institute of Physics and Chemistry ＆ Graduate University Chinese Academy of Sciences Beijing 100190 China

2-Ureido-4[1H]-pyrimidinone quadruple hydrogen-bonded assembly 1,1 containing N,N-dimethylaminophenyl moiety exhibits a sensitive response to fluoride anion and lead cation. Spectroscopic studies reveal that the presence of small amount of fluoride anions and lead cations can easily disassemble and intercalate 2-ureido- 4[ 1H]-pyri mi di none hydrogen-bonded supramolecular architectures.

关键词： 2-ureido-4[1H]-pyrimidinone assembly hydrogen bonds fluoride anion lead cation self-assembly

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Development of aryl-containing dipyrrolyldiketone difluoroboron complexes(BONEPYs):Tune the hydrogen bond o-C—H…F for fluoride recognition

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Chinese Chemical Letters 2020年第5期31卷 1317-1321页

作者： Xin-Dong Jiang Zhumei Shao Changliang Sun Shuai Yue Rong Shang Yohsuke Yamamoto College of Applied Chemistry Shenyang University of Chemical TechnologyShenyang 110142China Department of Chemistry Graduate School of ScienceHiroshima UniversityHigashi-Hiroshima 739-8526Japan

Dipyrrolyldiketone difluoroboron complexes(BONEPYs)were synthesized by condensation of the corresponding pyrroles and malonyl chloride followed by treatment with BF3·*** aryl-substituted pyrrole is introduced to form a cyclic system in order to investigate anion binding *** BONEPYs 1-3 the o-H of the aryl group forms hydrogen bonding with F to give a more table *** contrast,the intramolecular hydrogen-bonded BONEPY endo-4 is more stable than its exo *** adding F,the hydrogen bonds must be broken first to give 4·(3)*** to the electron-rich group(-OMe),the o-H of the phenyl group can hardly interact with F via hydrogen bonding to give the less stable complex4-(5)*** energy diffe rences between the different conformations were calculated using DFT methods,which is consistent to the experimental observations.

关键词： BONEPY Hydrogen bond Fluorescent dye fluoride anion Probe

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Amino-functionalized porous PDVB with high adsorption and regeneration performance for fluoride removal from water

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Green Chemical Engineering 2021年第2期2卷 224-232页

作者： Yuanyuan Huang Xianbiao Wang Yongfei Xu Shaojie Feng Jin Liu Huanting Wang Anhui Province International Research Center on Advanced Building Materials School of Materials Science and Chemical EngineeringAnhui Jianzhu UniversityHefei230601China Institute of Solid State Physics Chinese Academy of SciencesHefei230031China Anhui Institute of Building Science Research and Design Hefei230001China Department of Chemical Engineering Monash UniversityClaytonVictoria3800Australia

Excessive fluoride anions in drinking water are toxic to the health of human *** this article,an effective fluoride removal adsorbent on the basis of amino-functionalized porous polydivinylbenzene(PDVB)was prepared through low cost processes,which included solvothermal preparation of porous PDVB and subsequent surface *** obtained amino-functionalized porous PDVB(A-PDVB)has high surface area of 443 m2 g1 and high adsorption capacity towards fluoride anion up to 105.9 mg *** adsorbents surface area,the adsorption capacity per unit surface area of A-PDVB is 0.24 mg m2 which is more than 4 times of porous PDVB(0.058 mg m2).The enhanced adsorption performance of A-PDVB was due to amino groups electrostatic interaction coupled with hydrogen bond binding with fluoride *** addition,the aminofunctionalized porous PDVB could be regenerated in high efficiency under alkaline *** work not only exhibits the possibility of A-PDVB for application as an environment-friendly adsorbent for fluoride removal but also gives an insight into understanding mechanism of the fluoride anions adsorption onto aminofunctionalized porous PDVB.

关键词： Amino-functionalization Porous polydivinylbenzene(PDVB) Adsorption Regeneration fluoride anion

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Dimesitylborylphenyl substituted 1,3,4-oxadiazole:Synthesis,characterization and sensitivity to F^-

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Chinese Chemical Letters 2011年第5期22卷 599-602页

作者： Xiang Hong Li Bo Xu, Kang Le Lv Ai Qing Zhang College of Chemistry and Materials South-Central University for Nationalities Wuhan 430074 China

A new 1,3,4-oxadiazole compound with a dimesitylboryl group was synthesized and characterized by ~1H NMR,MS,element analysis and X-ray single-crystal *** exhibits good blue emission at 425 nm and high sensitivity to f... 详细信息

关键词： 1 3.4-Oxadiazole Dimesitylboryl fluoride anion Chemo-sensor

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