LDHs with different divalent metals (Zn-LDH, Mg-LDH and Ca-LDH) have been synthesized and produced calcined LDHs (Zn-CLDH, Mg-CLDH and Ca-CLDH) for borate removal. Based on XRD, SEM, BET, Al-27 NMR, CO2-TPD, and B-11 NMR, detailed characterization of different CLDHs before and after reaction with the boron species was systematically performed. The surface area, basicity and the particle charge of the different CLDHs, which are related to the hydration and regeneration, were markably influenced by the nature of the divalent metals. Transformation of crystal phases and the types of boron species adsorbed by the different CLDHs varied as time changed. The regeneration of Ca-CLDH required the shortest time. However, Ca-LDH decomposed to release Ca2+ ions, forming ettringite with borate. Zn-CLDH also rapidly transformed into Zn-LDH. During this reconstruction, B(OH)(4)(-) was intercalated into the interlayer of ZnLDHs, which is the predominant mechanism of borate removal by Zn-CLDH. Increase in the initial pH caused a competition between borate and OH- so that the removal efficiency of borate by Zn-CLDH decreased. For Mg-CLDH, surface complexation and electrostatic attraction were included in the first stage, immobilizing boric acid into mg(OH)(2) and attracting borate as interlayer anionic species into the new forming Mg-LDHs in the second stage. (C) 2015 Elsevier Inc. All rights reserved.