High-pressure and high-temperature transformation of Pb(II)-natrolite to Pb(II)-lawsonite

Junhyuck Im, Yongmoon Lee, Douglas A. Blom, Thomas Vogt, Yongjae Lee

Research output: Contribution to journalArticle

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Abstract

We report on high-pressure and high-temperature chemical transformations of Pb2+-exchanged natrolite (Pb-NAT, Pb8Al16Si24O80·16H2O) using a combination of in situ synchrotron X-ray powder diffraction and ex situ HAADF-STEM real space imaging. Three high-pressure polymorphs of natrolites (Pb-NAT-I, II, III) are observed via step-wise pressure-induced hydrations (PIH) up to 4.5 GPa, during which the number of H2O molecules located inside the natrolite channel increases from 16 to 40 H2O per unit-cell. At 4.5 GPa after heating the high-pressure Pb-NAT-III phase at 200 °C a reconstructive phase transits into a lawsonite phase (Pb-LAW, Pb4Al8Si8O28(OH)8·4H2O) with an orthorhombic space group Pbnm and a = 5.8216(9), b = 9.114(1) and c = 13.320(1) Å is observed. The structure of the recovered Pb-LAW phase was characterized using Rietveld refinement of the in situ synchrotron X-ray powder diffraction data and HAADF-STEM real space imaging. In the recovered Pb-LAW phase the Pb2+ content is close to 42 wt% and as bond valence approximations reveal the Pb2+ cations are more tightly coordinated to the framework oxygen atoms than originally in the natrolite phase.

Original languageEnglish
Pages (from-to)1622-1630
Number of pages9
JournalDalton Transactions
Volume45
Issue number4
DOIs
Publication statusPublished - 2016 Jan 1

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Synchrotrons
X ray powder diffraction
Imaging techniques
Temperature
Rietveld refinement
Polymorphism
Hydration
Cations
Oxygen
Heating
Atoms
Molecules
natrolite
N-acetyltalosaminuronic acid

All Science Journal Classification (ASJC) codes

  • Inorganic Chemistry

Cite this

Im, Junhyuck ; Lee, Yongmoon ; Blom, Douglas A. ; Vogt, Thomas ; Lee, Yongjae. / High-pressure and high-temperature transformation of Pb(II)-natrolite to Pb(II)-lawsonite. In: Dalton Transactions. 2016 ; Vol. 45, No. 4. pp. 1622-1630.
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High-pressure and high-temperature transformation of Pb(II)-natrolite to Pb(II)-lawsonite. / Im, Junhyuck; Lee, Yongmoon; Blom, Douglas A.; Vogt, Thomas; Lee, Yongjae.

In: Dalton Transactions, Vol. 45, No. 4, 01.01.2016, p. 1622-1630.

Research output: Contribution to journalArticle

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T1 - High-pressure and high-temperature transformation of Pb(II)-natrolite to Pb(II)-lawsonite

AU - Im, Junhyuck

AU - Lee, Yongmoon

AU - Blom, Douglas A.

AU - Vogt, Thomas

AU - Lee, Yongjae

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AB - We report on high-pressure and high-temperature chemical transformations of Pb2+-exchanged natrolite (Pb-NAT, Pb8Al16Si24O80·16H2O) using a combination of in situ synchrotron X-ray powder diffraction and ex situ HAADF-STEM real space imaging. Three high-pressure polymorphs of natrolites (Pb-NAT-I, II, III) are observed via step-wise pressure-induced hydrations (PIH) up to 4.5 GPa, during which the number of H2O molecules located inside the natrolite channel increases from 16 to 40 H2O per unit-cell. At 4.5 GPa after heating the high-pressure Pb-NAT-III phase at 200 °C a reconstructive phase transits into a lawsonite phase (Pb-LAW, Pb4Al8Si8O28(OH)8·4H2O) with an orthorhombic space group Pbnm and a = 5.8216(9), b = 9.114(1) and c = 13.320(1) Å is observed. The structure of the recovered Pb-LAW phase was characterized using Rietveld refinement of the in situ synchrotron X-ray powder diffraction data and HAADF-STEM real space imaging. In the recovered Pb-LAW phase the Pb2+ content is close to 42 wt% and as bond valence approximations reveal the Pb2+ cations are more tightly coordinated to the framework oxygen atoms than originally in the natrolite phase.

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