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2017 Fiscal Year Annual Research Report

Design of functionalized adsorbents for simultaneous removal of fluoride and arsenite from waters

Research Project

Project/Area Number 16F16082
Research InstitutionKyushu University

Principal Investigator

笹木 圭子  九州大学, 工学研究院, 教授 (30311525)

Co-Investigator(Kenkyū-buntansha) SUBBAIAH MUTHU PRABHU  九州大学, 工学(系)研究科(研究院), 外国人特別研究員
Project Period (FY) 2016-10-07 – 2019-03-31
KeywordsSucrose-derived carbon . / Oxyhydroxide materials / MOF-like materials / Arsenite / Arsenate / Fluoride / Binary solution / Adsorption
Outline of Annual Research Achievements

The adsorbents, ZrOOH, LaOOH, ZrxLa1-xOOH and sucrose-derived porous carbon (PSC) doped PSC-ZrxLa1-xOOH were prepared by chemical co-precipitation method and utilized for adsorption of F- and AsO33- from single/binary solutions. The mechanism of adsorption can be interpreted based on the HSAB principle, where the bimetallic oxyhydroxides become “soft acids”, while La3+ and Zr4+ are categorized as “hard acids”. Moreover, the PSC-ZrxLa1-xOOH adsorbent demonstrated high selectivity for AsO33- in the co-existence of other ions in a triple component system. Instead of PSC, a biopolymer, namely chitosan (CS) was used as a supporting material which possesses surface rich O- and N-containing functional groups such as -OH and -NH2, useful for bonding transition metal ions through a chelation mechanism which helps to enhance the adsorption capacity of several toxic ions. Chemical precipitation method was employed to synthesize ZrOOH, AlOOH, ZrxAl1-xOOH and CS@ ZrxAl1-xOOH and the resulting material showed high removal efficiency of simultaneous adsorption of AsO33- and F-. Also, the SPC@La-oxalate complex was prepared, where oxalate has been used as an organic ligand, and the carbonaceous biomass has been used as a doping material that is naturally carboxylate rich functional groups derived from sucrose biomass. The mechanism of AsO43- uptake was by ligand-exchange, chelation and electrostatic interaction between AsO43- and SPC@La-oxalate. The presence of other ions did not significantly affect the adsorption of AsO43-, which indicates the high selectivity.

Current Status of Research Progress
Current Status of Research Progress

2: Research has progressed on the whole more than it was originally planned.

Reason

MOF-like compounds have been synthesized including Zr and La as central metals, and their adsorption characteristics of arsenate, arsenite and fluoride have been revealed. The results can be well interpreted by HSAB theory. But their chemical stability in water, especially when they are utilized for adsorption of arsenate and fluoride, should be much improved. This is an action assignment to overcome.

Strategy for Future Research Activity

1.Graphene based magnetic nanocomposites for functionalized biopolymer for simultaneous adsorption of F- and AsO33-.
2.Synthesize of ligand-functionalized biopolymer for simultaneous adsorption of both F- and AsO33-.
3.Surfactant assisted mixed oxide onto biochar for simultaneous adsorption of F- and AsO33-.
4.Preparation of magnetic coated ZrO2 @polyamidoamine (PAMAM) dendrimer for F- and AsO33- adsorption from single and binary systems
5.Evaluation of their uptake mechanism, and understanding of the reduction pathways by different analyses such as EXAFS and XPS.

  • Research Products

    (6 results)

All 2018 2017

All Journal Article (3 results) (of which Int'l Joint Research: 2 results,  Peer Reviewed: 3 results) Presentation (3 results) (of which Int'l Joint Research: 3 results)

  • [Journal Article] A mechanistic approach for the synthesis of carboxylate-rich carbonaceous biomass-doped lanthanum-oxalate nanocomplex for arsenate adsorption2018

    • Author(s)
      Prabhu, S.M; Chuaicham, C.; Sasaki, K.
    • Journal Title

      ACS Sustainable Chemistry & Engineering

      Volume: in perss Pages: in press

    • DOI

      10.1021/acssuschemeng.7b04678

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Synthesis of sucrose-derived porous carbon-doped ZrxLa1-xOOH materials and their superior performance for the simultaneous immobilization of arsenite and fluoride from binary systems2017

    • Author(s)
      Prabhu, S.M.; Koilraj, P.; Sasaki, K.
    • Journal Title

      Chemical Engineering Journal

      Volume: 325 Pages: 1-13

    • DOI

      10.1016/j.cej.2017.05.052

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Fabrication of chitosan-reinforced ZrxAl1-xOOH nanocomposites and their arsenite and fluoride depollution densities from single/binary systems2017

    • Author(s)
      Prabhu, S.M.; Sasaki, K
    • Journal Title

      ChemistrySelect

      Volume: 2 Pages: 6375-6387

    • DOI

      10.1002/slct.201701072

    • Peer Reviewed
  • [Presentation] Synthesis of amorphous carbon-doped mixed oxyhydroxides and their dual performance for arsenite and fluoride uptake performance from binary mixture solution2017

    • Author(s)
      S.M. Prabhu, P. Koilraj, K, Sasaki
    • Organizer
      ACS Asia-Pacific International Chapters Conference 2017
    • Int'l Joint Research
  • [Presentation] Mono-, di- and tri carboxylic acids mediated lanthanum based organic frameworks for efficient removal of arsenic from water2017

    • Author(s)
      S. Imamura, S.M. Prabhu, K. Sasaki
    • Organizer
      International Symposium on Earth Science and Technology 2017
    • Int'l Joint Research
  • [Presentation] Synthesis of biopolymer supported ZrxAl1-xOOH nanocomposites and their fluoride/arsenite depollution densities from single/binary systems2017

    • Author(s)
      S.M. Prabhu, K. Sasaki
    • Organizer
      Symposium on Biomaterials 2017
    • Int'l Joint Research

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Published: 2018-12-17  

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