Synthesis of modulator-driven highly stable zirconium-fumarate frameworks and mechanistic investigations of their arsenite and arsenate adsorption from aqueous solutions

Subbaiah Muthu Prabhu, Srinivasarao Kancharla, Chang Min Park, Keiko Sasaki

研究成果: ジャーナルへの寄稿記事

1 引用 (Scopus)

抄録

Here, we synthesized a modulator (benzoic acid (BA))-driven zirconium-fumaric acid (Zr-fum) metal-organic framework (MOF) and investigated in detail the adsorption mechanism of arsenic oxyanions (AsO43− and AsO33−) and their stability before and after adsorption from water. Without the support of the modulator, BA, Zr-fum formed an amorphous MOF due to the occurrence of quick precipitation of both zirconium and -fum. Various amounts of BA, 0-10 eq. to ZrCl4, were used to control the surface charge on the MOF nanoparticles, which directly corresponds to the colloid stability of the MOF and helps to obtain a defect-free Zr-fum MOF for high uptakes of AsO43− and AsO33− from water. With the concentration of 3 eq. BA, the adsorption capacities of both arsenic oxyanions on the Zr-fum MOF were found to be higher than those on other MOFs. The CHN analysis indicated that the excess of -fum present does not alter the adsorption densities of AsO43− and AsO33− on MOFs in addition to the negligible amount of BA except for the Zr-fum-10 eq. BA MOF where it is present in higher amounts, as confirmed by NMR studies. The physicochemical properties of the synthesized MOFs with/without the modulator support adsorbents before and after the adsorption of AsO43− and AsO33− were extensively characterized using several advanced instrumental techniques. The maximum uptake performance of AsO43− (1.159 mmol g−1) and AsO33− (1.121 mmol g−1) was obtained using the Langmuir adsorption isotherm. The adsorption of both AsO43− and AsO33− takes place by electrostatic interaction/complexation and ligand exchange with Zr-fum-5 eq. BA. In addition, the Zr-fum-5 eq. BA was recycled up to four times at a sustained efficiency after washing with 0.1 M NaOH. Owing to their high uptake capacities of AsO43− and AsO33−, the synthesized MOFs are expected to have potential applications as adsorbents for practical applications.

元の言語英語
ページ(範囲)2320-2332
ページ数13
ジャーナルCrystEngComm
21
発行部数14
DOI
出版物ステータス出版済み - 1 1 2019

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arsenates
Fumarates
Benzoic Acid
Benzoic acid
benzoic acid
Zirconium
Modulators
modulators
aqueous solutions
Metals
Adsorption
adsorption
acids
synthesis
Acids
metals
Arsenic
adsorbents
arsenic
Adsorbents

All Science Journal Classification (ASJC) codes

  • Chemistry(all)
  • Materials Science(all)
  • Condensed Matter Physics

これを引用

Synthesis of modulator-driven highly stable zirconium-fumarate frameworks and mechanistic investigations of their arsenite and arsenate adsorption from aqueous solutions. / Muthu Prabhu, Subbaiah; Kancharla, Srinivasarao; Park, Chang Min; Sasaki, Keiko.

:: CrystEngComm, 巻 21, 番号 14, 01.01.2019, p. 2320-2332.

研究成果: ジャーナルへの寄稿記事

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abstract = "Here, we synthesized a modulator (benzoic acid (BA))-driven zirconium-fumaric acid (Zr-fum) metal-organic framework (MOF) and investigated in detail the adsorption mechanism of arsenic oxyanions (AsO43− and AsO33−) and their stability before and after adsorption from water. Without the support of the modulator, BA, Zr-fum formed an amorphous MOF due to the occurrence of quick precipitation of both zirconium and -fum. Various amounts of BA, 0-10 eq. to ZrCl4, were used to control the surface charge on the MOF nanoparticles, which directly corresponds to the colloid stability of the MOF and helps to obtain a defect-free Zr-fum MOF for high uptakes of AsO43− and AsO33− from water. With the concentration of 3 eq. BA, the adsorption capacities of both arsenic oxyanions on the Zr-fum MOF were found to be higher than those on other MOFs. The CHN analysis indicated that the excess of -fum present does not alter the adsorption densities of AsO43− and AsO33− on MOFs in addition to the negligible amount of BA except for the Zr-fum-10 eq. BA MOF where it is present in higher amounts, as confirmed by NMR studies. The physicochemical properties of the synthesized MOFs with/without the modulator support adsorbents before and after the adsorption of AsO43− and AsO33− were extensively characterized using several advanced instrumental techniques. The maximum uptake performance of AsO43− (1.159 mmol g−1) and AsO33− (1.121 mmol g−1) was obtained using the Langmuir adsorption isotherm. The adsorption of both AsO43− and AsO33− takes place by electrostatic interaction/complexation and ligand exchange with Zr-fum-5 eq. BA. In addition, the Zr-fum-5 eq. BA was recycled up to four times at a sustained efficiency after washing with 0.1 M NaOH. Owing to their high uptake capacities of AsO43− and AsO33−, the synthesized MOFs are expected to have potential applications as adsorbents for practical applications.",
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T1 - Synthesis of modulator-driven highly stable zirconium-fumarate frameworks and mechanistic investigations of their arsenite and arsenate adsorption from aqueous solutions

AU - Muthu Prabhu, Subbaiah

AU - Kancharla, Srinivasarao

AU - Park, Chang Min

AU - Sasaki, Keiko

PY - 2019/1/1

Y1 - 2019/1/1

N2 - Here, we synthesized a modulator (benzoic acid (BA))-driven zirconium-fumaric acid (Zr-fum) metal-organic framework (MOF) and investigated in detail the adsorption mechanism of arsenic oxyanions (AsO43− and AsO33−) and their stability before and after adsorption from water. Without the support of the modulator, BA, Zr-fum formed an amorphous MOF due to the occurrence of quick precipitation of both zirconium and -fum. Various amounts of BA, 0-10 eq. to ZrCl4, were used to control the surface charge on the MOF nanoparticles, which directly corresponds to the colloid stability of the MOF and helps to obtain a defect-free Zr-fum MOF for high uptakes of AsO43− and AsO33− from water. With the concentration of 3 eq. BA, the adsorption capacities of both arsenic oxyanions on the Zr-fum MOF were found to be higher than those on other MOFs. The CHN analysis indicated that the excess of -fum present does not alter the adsorption densities of AsO43− and AsO33− on MOFs in addition to the negligible amount of BA except for the Zr-fum-10 eq. BA MOF where it is present in higher amounts, as confirmed by NMR studies. The physicochemical properties of the synthesized MOFs with/without the modulator support adsorbents before and after the adsorption of AsO43− and AsO33− were extensively characterized using several advanced instrumental techniques. The maximum uptake performance of AsO43− (1.159 mmol g−1) and AsO33− (1.121 mmol g−1) was obtained using the Langmuir adsorption isotherm. The adsorption of both AsO43− and AsO33− takes place by electrostatic interaction/complexation and ligand exchange with Zr-fum-5 eq. BA. In addition, the Zr-fum-5 eq. BA was recycled up to four times at a sustained efficiency after washing with 0.1 M NaOH. Owing to their high uptake capacities of AsO43− and AsO33−, the synthesized MOFs are expected to have potential applications as adsorbents for practical applications.

AB - Here, we synthesized a modulator (benzoic acid (BA))-driven zirconium-fumaric acid (Zr-fum) metal-organic framework (MOF) and investigated in detail the adsorption mechanism of arsenic oxyanions (AsO43− and AsO33−) and their stability before and after adsorption from water. Without the support of the modulator, BA, Zr-fum formed an amorphous MOF due to the occurrence of quick precipitation of both zirconium and -fum. Various amounts of BA, 0-10 eq. to ZrCl4, were used to control the surface charge on the MOF nanoparticles, which directly corresponds to the colloid stability of the MOF and helps to obtain a defect-free Zr-fum MOF for high uptakes of AsO43− and AsO33− from water. With the concentration of 3 eq. BA, the adsorption capacities of both arsenic oxyanions on the Zr-fum MOF were found to be higher than those on other MOFs. The CHN analysis indicated that the excess of -fum present does not alter the adsorption densities of AsO43− and AsO33− on MOFs in addition to the negligible amount of BA except for the Zr-fum-10 eq. BA MOF where it is present in higher amounts, as confirmed by NMR studies. The physicochemical properties of the synthesized MOFs with/without the modulator support adsorbents before and after the adsorption of AsO43− and AsO33− were extensively characterized using several advanced instrumental techniques. The maximum uptake performance of AsO43− (1.159 mmol g−1) and AsO33− (1.121 mmol g−1) was obtained using the Langmuir adsorption isotherm. The adsorption of both AsO43− and AsO33− takes place by electrostatic interaction/complexation and ligand exchange with Zr-fum-5 eq. BA. In addition, the Zr-fum-5 eq. BA was recycled up to four times at a sustained efficiency after washing with 0.1 M NaOH. Owing to their high uptake capacities of AsO43− and AsO33−, the synthesized MOFs are expected to have potential applications as adsorbents for practical applications.

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