skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Accelerated carbonation and structural transformation of blast furnace slag by mechanochemical alkali-activation

Journal Article · · Cement and Concrete Research
 [1];  [1];  [1];  [1];  [2];  [2];  [1]
  1. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
  2. Metna Corporation, Lansing, MI (United States)

Alternative cements and production routes are necessary to offset the considerable global CO2 emissions of Portland cement production. The combination of alkali-activation and mechanochemical milling in a CO2 rich atmosphere is a promising green direction for synthesizing cementitious material as it upcycles hazardous material (slag) while capturing wt% of CO2 during synthesis. We investigate the resulting structural transformations incurred during synthesis and hydration using a suite of characterization techniques including solid-state 27Al, 29Si, and 13C NMR. The local aluminosilicate network structure of the processed clinker is best described by a melilite-type structure. Upon hydration, the network polymerizes to form a calcium, sodium aluminosilicate hydrate gel. The synthesis route also creates various metastable carbonates and bicarbonates from captured CO2 and alkali-additives that transform into stable carbonate phases like calcite, aragonite, and gaylussite, after hydration. These findings indicate accelerated carbonation reactions occur during clinker production and demonstrates novelty as a green cement technology.

Research Organization:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Organization:
USDOE National Nuclear Security Administration (NNSA)
Grant/Contract Number:
AC52-07NA27344; SC0011960
OSTI ID:
1864118
Report Number(s):
LLNL-JRNL-811939; 1019022
Journal Information:
Cement and Concrete Research, Vol. 156, Issue na; ISSN 0008-8846
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

References (72)

Potential reduction of carbon emissions by performance improvement: A cement industry case study journal November 2016
MATPASS/CPMG: A sensitivity enhanced magic-angle spinning sideband separation experiment for disordered solids journal August 2012
Hydraulic Behavior of Mechanically and Chemically Activated Synthetic Merwinite journal September 2014
Solid-State NMR Study of the Role of H and Na in AB-Type Carbonate Hydroxylapatite journal December 2007
Hydrogen bonding induced distortion of CO 3 units and kinetic stabilization of amorphous calcium carbonate: results from 2D 13 C NMR spectroscopy journal January 2016
Acid resistance and corrosion protection potential of concrete prepared with alkali aluminosilicate cement journal November 2018
Elucidation of the Al/Si Ordering in Gehlenite Ca 2 Al 2 SiO 7 by Combined 29 Si and 27 Al NMR Spectroscopy/Quantum Chemical Calculations journal October 2012
Structure and properties of calcium aluminosilicate glasses journal May 1991
Modelling one- and two-dimensional solid-state NMR spectra: Modelling 1D and 2D solid-state NMR spectra journal December 2001
Recent advances in alkaline cement binders: A review journal August 2019
The Atomic-Level Structure of Cementitious Calcium Aluminate Silicate Hydrate journal May 2020
Structural roles of CO2 and [CO3]2− in fully polymerized sodium aluminosilicate melts and glasses journal February 1995
CO 2 Sequestration Potential of Steel Slags at Ambient Pressure and Temperature journal September 2008
Mechanochemical interaction of alkali metal metasilicates with carbon dioxide: 1. Absorption of CO2 and phase formation journal February 2008
13C chemical shift anisotropies for carbonate ions in cement minerals and the use of 13C, 27Al and 29Si MAS NMR in studies of Portland cement including limestone additions journal October 2013
An infrared and Raman study of carbonate glasses: implications for the structure of carbonatite magmas journal March 1995
Elucidating the Effect of Accelerated Carbonation on Porosity and Mechanical Properties of Hydrated Portland Cement Paste Using X-Ray Tomography and Advanced Micromechanical Testing journal April 2020
Conversion of Landfilled Ash into Hydraulic Cements under Different Environments journal January 2017
Structure and Crystallization of Alkaline-Earth Aluminosilicate Glasses: Prevention of the Alumina-Avoidance Principle journal April 2018
Carbon dioxide use in beneficiation of landfilled coal ash for hazardous waste immobilization journal April 2018
Monohydrocalcite in Comparison with Hydrated Amorphous Calcium Carbonate: Precipitation Condition and Thermal Behavior journal September 2011
Crystallo-chemical evolution of a crystal structure due to cationic substitution after the example of melilite journal July 1985
Changes in Structural and Electronic Properties of the Zeolite Framework Induced by Extraframework Al and La in H-USY and La( x )NaY:  A 29 Si and 27 Al MAS NMR and 27 Al MQ MAS NMR Study journal July 2000
A method of assessing solid state reactivity illustrated by thermal decomposition experiments on sodium bicarbonate journal May 1995
Aluminium triplets in dealuminated zeolites detected by 27Al NMR correlation spectroscopy journal April 2010
Proto-Calcite and Proto-Vaterite in Amorphous Calcium Carbonates journal October 2010
MAS-NMR studies of carbonate retention in a very wide range of Na2O-SiO2 glasses journal April 2020
A review on alkaline activation: new analytical perspectives [A review on alkaline activation: new analytical perspectives] journal August 2014
Alkali-activated slag characterization by scanning electron microscopy, X-ray microanalysis and nuclear magnetic resonance spectroscopy journal October 2020
Effectiveness of using CO 2 pressure to enhance the carbonation of Portland cement-fly ash-MgO mortars journal July 2016
27 Al and 29 Si Solid-State NMR Characterization of Calcium-Aluminosilicate-Hydrate journal January 2012
Chemical acceleration of a neutral granulated blast-furnace slag activated by sodium carbonate journal June 2015
Concrete calcium leaching at variable temperature: Experimental data and numerical model inverse identification journal June 2010
29 Si Chemical Shift Anisotropies in Calcium Silicates from High-Field 29 Si MAS NMR Spectroscopy journal April 2003
Nanostructure of CaO-(Na 2 O)-Al 2 O 3 -SiO 2 -H 2 O Gels Revealed by Multinuclear Solid-State Magic Angle Spinning and Multiple Quantum Magic Angle Spinning Nuclear Magnetic Resonance Spectroscopy journal December 2019
Observation of bicarbonate in calcite by NMR spectroscopy journal May 2006
Carbonation of cement-based materials: Challenges and opportunities journal September 2016
Layered double hydroxides modify the reaction of sodium silicate-activated slag cements journal June 2019
Effect of alkalis on fresh C–S–H gels. FTIR analysis journal March 2009
Hydrated double carbonates – A Raman and infrared spectroscopic study journal September 2007
Geopolymers and other alkali activated materials: why, how, and what? journal November 2013
Structural evolution of synthetic alkali-activated CaO-MgO-Na 2 O-Al 2 O 3 -SiO 2 materials is influenced by Mg content journal September 2017
Phase evolution of C-(N)-A-S-H/N-A-S-H gel blends investigated via alkali-activation of synthetic calcium aluminosilicate precursors journal November 2016
Alkali-activated slag cements produced with a blended sodium carbonate/sodium silicate activator journal April 2016
Differential thermal analysis of the decomposition of sodium bicarbonate and its simple double salts journal January 1966
Measurement methods of carbonation profiles in concrete: Thermogravimetry, chemical analysis and gammadensimetry journal August 2007
Carbon capture and storage using alkaline industrial wastes journal April 2012
Synthesis and characterization of alkali aluminosilicate hydraulic cement that meets standard requirements for general use journal January 2018
A NMR and molecular dynamics study of CO2-bearing basaltic melts and glasses journal December 2015
MAS NMR spectra of quadrupolar nuclei in disordered solids: The Czjzek model journal June 2008
Quantitative Analysis of Sodium Carbonate and Sodium Bicarbonate in Solid Mixtures Using Fourier Transform Infrared Spectroscopy (FT-IR) journal August 2013
Landfilled coal ash for carbon dioxide capture and its potential as a geopolymer binder for hazardous waste remediation journal August 2021
Reactivity and strength development of CO2 activated non-hydraulic calcium silicates journal January 1979
The negative emission potential of alkaline materials journal March 2019
Structure and reactivity of synthetic CaO-Al2O3-SiO2 glasses journal June 2019
MgO content of slag controls phase evolution and structural changes induced by accelerated carbonation in alkali-activated binders journal March 2014
Review on recent advances in CO2 utilization and sequestration technologies in cement-based materials journal November 2016
29Si and 27Al MAS-NMR of NaOH-Activated Blast-Furnace Slag journal September 1994
Transformation of meta-stable calcium silicate hydrates to tobermorite: reaction kinetics and molecular structure from XRD and NMR spectroscopy journal January 2009
29 Si Chemical Shift Anisotropies in Hydrated Calcium Silicates: A Computational Study journal April 2013
Carbon dioxide integration into alkali aluminosilicate cement particles for achievement of improved properties journal September 2018
Carbonate speciation in depolymerized and polymerized (alumino)silicate glasses: Constraints from 13C MAS and static NMR measurements and ab initio calculations journal February 2018
Generalized Structural Description of Calcium–Sodium Aluminosilicate Hydrate Gels: The Cross-Linked Substituted Tobermorite Model journal April 2013
Mechanochemical interaction of Ca silicate and aluminosilicate minerals with carbon dioxide journal August 2004
Rapid acquisition of data dense solid-state CPMG NMR spectral sets using multi-dimensional statistical analysis journal January 2018
Effect of pressure on the short-range structure and speciation of carbon in alkali silicate and aluminosilicate glasses and melts at high pressure up to 8 GPa: 13C, 27Al, 17O and 29Si solid-state NMR study journal March 2018
Two-dimensional magic-angle spinning isotropic reconstruction sequences for quadrupolar nuclei journal February 1996
Triple-Quantum Two-Dimensional 27 Al Magic Angle Nuclear Magnetic Resonance Study of the Aluminum Incorporation in Calcium Silicate Hydrates journal November 1998
Sintering and devitrification of glass-powder compacts in the akermanite–gehlenite system journal February 2013
Speedy Component Resolution: An Improved Tool for Processing Diffusion-Ordered Spectroscopy Data journal May 2008
Review on carbonation curing of cement-based materials journal October 2017
Solubility and solution mechanisms of C–O–H volatiles in silicate melt with variable redox conditions and melt composition at upper mantle temperatures and pressures journal October 2011