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Complexation of As(Ⅲ)by phosphonate ligands in aqueous fluids:Thermodynamic behavior,chemical binding forms and sequestering abilities

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Journal of Environmental Sciences 2020年第8期32卷 100-110页

作者： Donatella Chillè Donatella Aiello Giuseppa Ida Grasso Ottavia Giuffrè Anna Napoli Carmelo Sgarlata Claudia Foti Dipartimento di Scienze Chimiche BiologicheFarmaceutiche ed AmbientaliUniversitàdi MessinaViale F.Stagno d’Alcontres 3198166 MessinaItaly Dipartimento di Chimica e Tecnologie Chimiche Universitàdella CalabriaVia P.Bucci87036 Arcavacata di Rende(CS)Italy Dipartimento di Scienze Chimiche Universitàdegli Studi di CataniaViale A.Doria 695125 CataniaItaly

In recent years,the contamination of water by arsenic reached alarming levels in many countries of the world,attracting the interest of many researchers engaged in testing methodologies able to remove this harmful *** important aspect that must be taken into consideration is the possibility to find arsenic in different chemical forms which could require different approaches for its *** this aim,a speciation analysis appears to be crucial for better understanding the behavior of arsenic species in aqueous solutions,especially in presence of compounds with marked chelating *** can be identified as good sequestering agents and,at this purpose,this manuscript intends to investigate the interaction of As(Ⅲ)with three phosphonic acids derived from nitrilotriacetic acid(NTA)by replacements of one(N-(Phosphonomethyl)iminodiacetic acid,NTAP),two(N,N-Bis-(phosphonomethyl)glycine,NTA2P)and three(Nitrilotri(methylphosphonic acid),NTA3P)carboxylic groups with the same number of phosphonate *** in-depth potentiometric and calorimetric investigation allowed to determine speciation models featured by simple ML,MLH i and ML(OH)species.A complete thermodynamic characterization of the systems is reported together with the definition of coordination mode by mass spectrometry *** the light of the speciation models,the possibility of using these ligands in arsenic removal techniques was assessed by determining the pL 0.5(the concentration of ligand able to remove the 50%of metal ion present in trace).All ligands show a good sequestering ability,in particular under the conditions of fresh water,following the trend NTA3P>NTA2P>NTAP.

关键词： phosphonate ligands Arsenic Thermodynamic interaction parameters Sequestering ability

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Luminescence study of europium(III) tris(β-diketonato)/phosphonate complexes in chloroform

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Journal of Rare Earths 2008年第2期26卷 185-191页

作者： Stefan Lis Zbigniew Piskula Krzysztof Staninski Sayaka Tamaki Masayuki Inoue Yuko Hasegawa Department of Rare Earths Faculty of Chemistry Adam Mickiewicz University Grunwaldzka 6 Department of Chemistry Faculty of Science Science University of Tokyo

The extraction of Eu（Ⅲ） with β-diketone, HA, and monodentate or bidentate Lewis bases, B, into chloroform and the luminescence properties of the extracted species were studied. Pivaloyltrifluoroacetone, Hpta, and 2-thenoyltfifluoroacetone, Htta, were used as the β-diketones. The Lewis bases, B, were tetraethyl methylene diphosphonate, POPO, which was bidentate, and diethyl benzylphosphonate, PhPO which was monodentate. Based on the extraction data, the stability constants, log β, of the first complexes between tfis（β-diketonato）Eu（Ⅲ） and the phosphonate, EuA3B, were determined to be 6.0 for the POPO complex and 3.40 for the PhPO complex. The Eu（Ⅲ） luminescence intensity in the EuA3POPO was larger than EuA3 where A was either pta or tta at similar concentrations of Eu（Ⅲ）, while that in Eu（pta）3PhPO was stronger than EuA3; however, in Eu（tta）3PhPO, it was weaker than Eu（tta）3. The POPO functions as a sensitizer, and the PhPO functions as a quencher for the tta chelate and as a sensitizer for the pta chelate. From the lifetime and quantum yield, φ, of the Eu（Ⅲ） luminescence in the complexes as well as the observation of the extractability of Eu（Ⅲ） with the Hpta and the phosphonates and of the luminescence spectra of the complexes, it was confirmed that the extraction of Eu（Ⅲ） was remarkably enhanced with a β-diketonate and a strong Lewis base, and also the ternary complex that was formed as the extracted species, showed luminescence enhancement. This phenomenon may be due the formation of a strong bond between the Eu（Ⅲ） and the strong Lewis base leading to more hydrophobicity in the extracted species and also to more effective energy transfer from the Lewis base to the Eu（Ⅲ）. It was not significant whether the donor atoms were N or O.

关键词： tris(β-diketonato)Eu(Ⅲ) extraction luminescence phosphonate ligands rare earths

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