Ca-rich Ca-Al-oxide, high-temperature-stable sorbents prepared from hydrotalcite precursors: Synthesis, characterization, and CO2 capture capacity

Po Hsueh Chang, Yen Po Chang, San-Yuan Chen*, Ching Tsung Yu, Yau Pin Chyou

*Corresponding author for this work

Research output: Contribution to journalArticle

60 Scopus citations

Abstract

We present the design and synthesis of Ca-rich Ca-Al-O oxides, with Ca 2+/Al3+ ratios of 1:1, 3:1, 5:1, and 7:1, which were prepared by hydrothermal decomposition of coprecipitated hydrotalcite-like Ca-Al-CO3 precursors, for high-temperature CO2 adsorption at 500-700 °C. In situ X-ray diffraction measurements indicate that the coprecipitated, Ca-rich, hydrotalcite-like powders with Ca2+/Al 3+ ratios of 5:1 and 7:1 contained Ca(OH)2 and layered double hydroxide (LDH) phases. Upon annealing, LDH was first destroyed at approximately 200 °C to form an amorphous matrix, and then at 450-550 °C, the Ca(OH)2 phase was converted into a CaO matrix with incorporated Al3+ to form a homogeneous solid solution without a disrupted lattice structure. CaO nanocrystals were grown by thermal treatment of the weakly crystalline Ca-Al-O oxide matrix. Thermogravimetric analysis indicates that a CO2 adsorption capacity of approximately 51 wt. % can be obtained from Ca-rich Ca-Al-O oxides prepared by calcination of 7:1 Ca-Al-CO3 LDH phases at 600-700 °C. Furthermore, a relatively high CO2 capture capability can be achieved, even with gas flows containing very low CO2 concentrations (CO2/N 2=10 %). Approximately 95.6 % of the initial CO2 adsorption capacity of the adsorbent is retained after 30 cycles of carbonation-calcination. TEM analysis indicates that carbonation-promoted CaCO3 formation in the Ca-Al-O oxide matrix at 600 °C, but a subsequent desorption in N2 at 700 °C, caused the formation CaO nanocrystals of approximately 10 nm. The CaO nanocrystals are widely distributed in the weakly crystalline Ca-Al-O oxide matrix and are present during the carbonation-calcination cycles. This demonstrates that Ca-Al-O sorbents that developed through the synthesis and calcination of Ca-rich Ca-Al LDH phases are suitable for long-term cyclic operation in severe temperature environments.

Original languageEnglish
Pages (from-to)1844-1851
Number of pages8
JournalChemSusChem
Volume4
Issue number12
DOIs
StatePublished - 16 Dec 2011

Keywords

  • adsorption
  • carbon storage
  • coprecipitation
  • hydrothermal synthesis
  • layered compounds

Fingerprint Dive into the research topics of 'Ca-rich Ca-Al-oxide, high-temperature-stable sorbents prepared from hydrotalcite precursors: Synthesis, characterization, and CO<sub>2</sub> capture capacity'. Together they form a unique fingerprint.

  • Cite this