TY - JOUR
T1 - Activation and local structural stability during the thermal decomposition of Mg/Al-hydrotalcite by total neutron scattering
AU - Mourad, Maurice C.D.
AU - Mokhtar, Mohamed
AU - Tucker, Matthew G.
AU - Barney, Emma R.
AU - Smith, Ronald I.
AU - Alyoubi, Abdulrahaman O.
AU - Basahel, Sulaiman N.
AU - Shaffer, Milo S.P.
AU - Skipper, Neal T.
PY - 2011/10/21
Y1 - 2011/10/21
N2 - The activation of synthetic hydrotalcite, the carbonated layered double hydroxide (LDH) with ratio Mg2+/Al3+ = 3 and structural formula [Mg6Al2(OH)16]2+· CO3
2-n(H2O), has been investigated using neutron and X-ray diffraction. In situ neutron diffraction was used to follow the structural phase transformations during the thermal decomposition (calcination) of hydrotalcite under vacuum in the temperature range 298-723 K, and during which the residual gas evolved by the sample was analysed by mass spectrometry. Detailed structural information of the LDH and mixed metal oxides (MMOs) was extracted from both the Bragg peaks and the total scattering. These two analysis techniques provide complementary insight into the relevant transition mechanisms, since Bragg diffraction originates from long-range periodicities within the samples while total scattering reveals the subtleties of the local atomic environment. This latter information is particularly important for our understanding of catalytic activity since it elucidates the local metal coordination. We find that, during the calcination process, the local environment around the metal centres is robust, as the various stages during the phase transition have identical local structures. The implications of these new results for the nature of the MMOs is discussed in relation to the well-studied, reverse, rehydration reaction, and the high propensity of trivalent Al ions to migrate to tetrahedrally-coordinated lattice sites.
AB - The activation of synthetic hydrotalcite, the carbonated layered double hydroxide (LDH) with ratio Mg2+/Al3+ = 3 and structural formula [Mg6Al2(OH)16]2+· CO3
2-n(H2O), has been investigated using neutron and X-ray diffraction. In situ neutron diffraction was used to follow the structural phase transformations during the thermal decomposition (calcination) of hydrotalcite under vacuum in the temperature range 298-723 K, and during which the residual gas evolved by the sample was analysed by mass spectrometry. Detailed structural information of the LDH and mixed metal oxides (MMOs) was extracted from both the Bragg peaks and the total scattering. These two analysis techniques provide complementary insight into the relevant transition mechanisms, since Bragg diffraction originates from long-range periodicities within the samples while total scattering reveals the subtleties of the local atomic environment. This latter information is particularly important for our understanding of catalytic activity since it elucidates the local metal coordination. We find that, during the calcination process, the local environment around the metal centres is robust, as the various stages during the phase transition have identical local structures. The implications of these new results for the nature of the MMOs is discussed in relation to the well-studied, reverse, rehydration reaction, and the high propensity of trivalent Al ions to migrate to tetrahedrally-coordinated lattice sites.
UR - http://www.scopus.com/inward/record.url?scp=80053313870&partnerID=8YFLogxK
U2 - 10.1039/c1jm11530h
DO - 10.1039/c1jm11530h
M3 - Article
AN - SCOPUS:80053313870
SN - 0959-9428
VL - 21
SP - 15479
EP - 15485
JO - Journal of Materials Chemistry
JF - Journal of Materials Chemistry
IS - 39
ER -