Transformation of Gibbsite to Boehmite in Caustic Aqueous Solution at Hydrothermal Conditions

Zhang, Xin; Cui, Wenwen; Hu, Jian Z.; Wang, Hsiu-Wen; Prange, Micah P.; Wan, Chuan; Jaegers, Nicholas R.; Zong, Meirong; Zhang, Hailin; Pearce, Carolyn I.; Li, Ping; Wang, Zheming; Clark, Sue B.; Rosso, Kevin M.

doi:10.1021/acs.cgd.9b00468

Transformation of Gibbsite to Boehmite in Caustic Aqueous Solution at Hydrothermal Conditions

Journal Article · Wed Oct 02 00:00:00 EDT 2019 · Crystal Growth & Design

DOI:https://doi.org/10.1021/acs.cgd.9b00468· OSTI ID:1577095

Zhang, Xin ^[1]; Cui, Wenwen ^[2]; ^[1]; Wang, Hsiu-Wen ^[3]; ^[1]; Wan, Chuan ^[4]; Jaegers, Nicholas R. ^[1]; Zong, Meirong ^[4]; Zhang, Hailin ^[2]; Pearce, Carolyn I. ^[1]; Li, Ping ^[4]; ^[1]; Clark, Sue B. ^[1]; ^[1]

BATTELLE (PACIFIC NW LAB)
Chinese Academy of Sciences
OAK RIDGE NATIONAL LAB
UNIVERSITY PROGRAMS

Phase transformations among aluminum (oxyhydr)oxide minerals play important roles across a wide range of natural and industrial settings. In highly caustic aqueous solutions, uncertainty persists regarding whether solid-state or dissolution-reprecipitation pathways dominate. We explored transformation of gibbsite [a Al(OH)3] to boehmite (? AlOOH) in caustic NaOH solution at hydrothermal conditions as a function of temperature, Al(III) and NaOH concentrations, and reaction time. Comparison of detailed structural and morphological solids characterization by XRD, SEM/TEM, AFM, Raman spectroscopy, and high field 27Al MAS NMR to predictions from equilibrium thermodynamics calculations suggests the critical importance of dissolution-reprecipitation across our range of system conditions. The yield and physical properties of the boehmite product was found to be sensitive to the hydrothermal treatment temperature and the Al/OH- ratio, controlled by the loading of gibbsite with respect to NaOH. Experiments at lower Al/OH- ratios (e.g., 0.64) indicate that the dissolution of the gibbsite reaches an aqueous aluminate saturation state sufficient to overcome the nucleation barrier for boehmite. Higher Al/OH- ratios (e.g., 3.2) are found to slow the phase transformation, leaving residual unreacted gibbsite in the final product. Higher temperatures appear to improve the phase transformation rate, but also typically yield smaller sized boehmite particles. Particle morphological analyses compared to thermodynamic expectations suggest an important role of kinetics at mineral/solution interfaces, both in the gibbsite dissolution rate as well as the growth rate of boehmite nanocrystals.

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Interfacial Dynamics in Radioactive Environments and Materials (IDREAM); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE

DOE Contract Number:: AC05-76RL01830

OSTI ID:: 1577095

Report Number(s):: PNNL-SA-146423

Journal Information:: Crystal Growth & Design, Journal Name: Crystal Growth & Design Journal Issue: 10 Vol. 19

Country of Publication:: United States

Language:: English

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