Carbonation of Hydrous Materials at the Molecular Level: A Time of Flight-Secondary Ion Mass Spectrometry, Raman and Density Functional Theory Study

Giovanni L Pesce, Ian W Fletcher, Robert Grant, Marco Molinari, Stephen C Parker, Richard J Ball

Research output: Contribution to journalArticle

6 Citations (Scopus)

Abstract

Carbonation of hydrous minerals such as calcium hydroxide (Ca(OH)2) is an important process in environmental and industrial applications for the construction industry, geological disposal repositories for nuclear waste, and green technologies for carbon capture. Although the role of ions during the carbonation mechanism of Ca(OH)2 is still unclear, we identified the exchange of ions during the dissolution and precipitation process, by determining the change in isotopic composition of carbonation products using time-of-flight-secondary ion mass spectrometry. Our samples of pure Ca(18OH)2 carbonated in air were characterized using scanning electron microscopy and Raman spectroscopy, aided by density functional theory calculations. Our results show that the carbonation process at high pH is a two-stage mechanism. The first stage occurs in a short time after Ca(18OH)2 is exposed to air and involved the dissolution of surface Ca ions and hydroxyl 18OH groups, which reacts directly with dissolved CO2, leading to 1/3 of 18O in the oxygen content of carbonate phases. The second stage occurs within 24 h of exposure allowing a rebalance of the oxygen isotopic composition of the carbonate phases with a higher content of 16O.
LanguageEnglish
Pages1036-1044
Number of pages9
JournalCrystal Growth and Design
Volume17
Issue number3
Early online date2 Feb 2017
DOIs
StatusPublished - 1 Mar 2017

Fingerprint

Carbonation
Secondary ion mass spectrometry
secondary ion mass spectrometry
Density functional theory
density functional theory
Carbonates
carbonates
dissolving
construction industry
Ions
ions
Dissolution
air
disposal
radioactive wastes
Geological repositories
oxygen
Oxygen
Radioactive Waste
Environmental technology

Cite this

Carbonation of Hydrous Materials at the Molecular Level : A Time of Flight-Secondary Ion Mass Spectrometry, Raman and Density Functional Theory Study. / Pesce, Giovanni L; Fletcher, Ian W; Grant, Robert; Molinari, Marco; Parker, Stephen C; Ball, Richard J.

In: Crystal Growth and Design, Vol. 17, No. 3, 01.03.2017, p. 1036-1044.

Research output: Contribution to journalArticle

@article{c7be5db5da4a459e8d760ccad63e8f9b,
title = "Carbonation of Hydrous Materials at the Molecular Level: A Time of Flight-Secondary Ion Mass Spectrometry, Raman and Density Functional Theory Study",
abstract = "Carbonation of hydrous minerals such as calcium hydroxide (Ca(OH)2) is an important process in environmental and industrial applications for the construction industry, geological disposal repositories for nuclear waste, and green technologies for carbon capture. Although the role of ions during the carbonation mechanism of Ca(OH)2 is still unclear, we identified the exchange of ions during the dissolution and precipitation process, by determining the change in isotopic composition of carbonation products using time-of-flight-secondary ion mass spectrometry. Our samples of pure Ca(18OH)2 carbonated in air were characterized using scanning electron microscopy and Raman spectroscopy, aided by density functional theory calculations. Our results show that the carbonation process at high pH is a two-stage mechanism. The first stage occurs in a short time after Ca(18OH)2 is exposed to air and involved the dissolution of surface Ca ions and hydroxyl 18OH groups, which reacts directly with dissolved CO2, leading to 1/3 of 18O in the oxygen content of carbonate phases. The second stage occurs within 24 h of exposure allowing a rebalance of the oxygen isotopic composition of the carbonate phases with a higher content of 16O.",
author = "Pesce, {Giovanni L} and Fletcher, {Ian W} and Robert Grant and Marco Molinari and Parker, {Stephen C} and Ball, {Richard J}",
year = "2017",
month = "3",
day = "1",
doi = "10.1021/acs.cgd.6b01303",
language = "English",
volume = "17",
pages = "1036--1044",
journal = "Crystal Growth and Design",
issn = "1528-7483",
publisher = "American Chemical Society",
number = "3",

}

TY - JOUR

T1 - Carbonation of Hydrous Materials at the Molecular Level

T2 - Crystal Growth and Design

AU - Pesce, Giovanni L

AU - Fletcher, Ian W

AU - Grant, Robert

AU - Molinari, Marco

AU - Parker, Stephen C

AU - Ball, Richard J

PY - 2017/3/1

Y1 - 2017/3/1

N2 - Carbonation of hydrous minerals such as calcium hydroxide (Ca(OH)2) is an important process in environmental and industrial applications for the construction industry, geological disposal repositories for nuclear waste, and green technologies for carbon capture. Although the role of ions during the carbonation mechanism of Ca(OH)2 is still unclear, we identified the exchange of ions during the dissolution and precipitation process, by determining the change in isotopic composition of carbonation products using time-of-flight-secondary ion mass spectrometry. Our samples of pure Ca(18OH)2 carbonated in air were characterized using scanning electron microscopy and Raman spectroscopy, aided by density functional theory calculations. Our results show that the carbonation process at high pH is a two-stage mechanism. The first stage occurs in a short time after Ca(18OH)2 is exposed to air and involved the dissolution of surface Ca ions and hydroxyl 18OH groups, which reacts directly with dissolved CO2, leading to 1/3 of 18O in the oxygen content of carbonate phases. The second stage occurs within 24 h of exposure allowing a rebalance of the oxygen isotopic composition of the carbonate phases with a higher content of 16O.

AB - Carbonation of hydrous minerals such as calcium hydroxide (Ca(OH)2) is an important process in environmental and industrial applications for the construction industry, geological disposal repositories for nuclear waste, and green technologies for carbon capture. Although the role of ions during the carbonation mechanism of Ca(OH)2 is still unclear, we identified the exchange of ions during the dissolution and precipitation process, by determining the change in isotopic composition of carbonation products using time-of-flight-secondary ion mass spectrometry. Our samples of pure Ca(18OH)2 carbonated in air were characterized using scanning electron microscopy and Raman spectroscopy, aided by density functional theory calculations. Our results show that the carbonation process at high pH is a two-stage mechanism. The first stage occurs in a short time after Ca(18OH)2 is exposed to air and involved the dissolution of surface Ca ions and hydroxyl 18OH groups, which reacts directly with dissolved CO2, leading to 1/3 of 18O in the oxygen content of carbonate phases. The second stage occurs within 24 h of exposure allowing a rebalance of the oxygen isotopic composition of the carbonate phases with a higher content of 16O.

UR - https://doi.org/10.1021/acs.cgd.6b01303

U2 - 10.1021/acs.cgd.6b01303

DO - 10.1021/acs.cgd.6b01303

M3 - Article

VL - 17

SP - 1036

EP - 1044

JO - Crystal Growth and Design

JF - Crystal Growth and Design

SN - 1528-7483

IS - 3

ER -