Precision Calcination Mechanism of CaCO3 to High‐Porosity Nanoscale CaO CO2 Sorbent Revealed by Direct In Situ Observations

Author:

Martinez Jenny1,Wardini Jenna L.1,Zheng Xueli23,Moghimi Lauren23,Rakowsky Jason4,Means Jonathan1,Guo Huiming1,Kuzmenko Ivan5,Ilavsky Jan5,Zhang Fan6,Dholabhai Pratik P.4,Dresselhaus‐Marais Leora23,Bowman William J.1ORCID

Affiliation:

1. Department of Materials Science and Engineering University of California Irvine Irvine CA 92697 USA

2. Department of Materials Science and Engineering Stanford University Stanford CA 94305 USA

3. SLAC National Accelerator Laboratory Menlo Park CA 94025 USA

4. School of Physics and Astronomy Rochester Institute of Technology New York NY 14623 USA

5. X‐ray Science Division Argonne National Laboratory Lemont IL 60439 USA

6. Materials Measurement Science Division National Institute of Standards and Technology Gaithersburg MD 20899 USA

Abstract

AbstractDeploying energy storage and carbon capture at scale is hindered by the substantial endothermic penalty of decomposing CaCO3 to CaO and CO2, and the rapid loss of CO2 absorption capacity by CaO sorbent particles due to sintering at the high requisite decomposition temperatures. The decomposition reaction mechanism underlying sorbent deactivation remains unclear at the atomic level and nanoscale due to past reliance on postmortem characterization methods with insufficient spatial and temporal resolution. Thus, elucidating the important CaCO3 decomposition reaction pathway requires direct observation by time‐resolved (sub‐)nanoscale methods. Here, chemical and structural dynamics during the decomposition of CaCO3 nanoparticles to nanoporous CaO particles comprising high‐surface‐area CaO nanocrystallites are examined. Comparing in situ transmission electron microscopy (TEM) and synchrotron X‐ray diffraction experiments gives key insights into the dynamics of nanoparticle calcination, involving anisotropic CaCO3 thermal distortion before conversion to thermally dilated energetically stable CaO crystallites. Time‐resolved TEM uncovered a novel CaO formation mechanism involving heterogeneous nucleation at extended CaCO3 defects followed by sweeping reaction front motion across the initial CaCO3 particle. These observations clarify longstanding, yet incomplete, reaction mechanisms and kinetic models lacking accurate information about (sub‐)nanoscale dynamics, while also demonstrating calcination of CaCO3 without sintering through rapid heating and precise temperature control.

Funder

National Science Foundation

American Chemical Society Petroleum Research Fund

Publisher

Wiley

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