Tuning the Nature of the Anion in Hydrated Layered
Double Hydroxides for H2 Production under Ionizing Radiation
Version 2 2018-09-20, 18:49
Version 1 2018-09-20, 18:33
Posted on 2018-09-20 - 18:49
Layered double hydroxides (LDHs)
are adsorbent materials able to
store significant amounts of anionic radionuclides under various levels
of hydrations. In view of this storage application, it is crucial
to understand their evolution under ionizing radiation, particularly
as a function of their hydration state. We thus synthesized four LDHs,
with Mg/Al molar ratio ∼3.5 and four different anions: NO3–, CO32–, ClO4–, and Cl– chosen for
their contrasted behavior toward ionizing radiation. For all these
materials, the initial interlamellar distance increases slightly within
the first step of relative humidity (RH), 0–3%, and remains
constant in the 3–74% RH range. Infrared spectroscopy reveals
a lowering of the anion symmetry when it is confined in LDHs, caused
by the interaction with surface OH groups and water molecules together
with a decrease of degrees of freedom upon confinement. When RH increases,
the environment of the anions becomes more and more symmetric. Under
ionizing radiation, the nature of the anion in the interlamellar space
and the hydration state control the H2 production. The LDH containing nitrate anions leads to low H2 yields,
as nitrate anions scavenge precursors of dihydrogen. Materials containing
perchlorate (inert toward ionizing radiation) and carbonate (hydroxyl
scavenger) anions lead to very similar H2 yields, which
increase in the 0–3% RH range and then remain stable in the
3–74% range, with a maximum value approximately half of that
obtained for bulk water. This shows that the material itself contains
hydroxyl scavengers. The sample containing chloride anions produces
the highest H2 amounts, with H2 yields twice
higher than the yield measured in bulk water. This peculiar behavior
can be linked to specific reactions involving confined chloride anions.
This work shows that the anion of the LDH sample can be selected depending
on the applications.
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Lainé, Maxime; Liao, Yuanyuan; Varenne, Fanny; Picot, Pierre; Michot, Laurent J.; Barruet, Elodie; et al. (2018). Tuning the Nature of the Anion in Hydrated Layered
Double Hydroxides for H2 Production under Ionizing Radiation. ACS Publications. Collection. https://doi.org/10.1021/acsanm.8b01240
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AUTHORS (12)
ML
Maxime Lainé
YL
Yuanyuan Liao
FV
Fanny Varenne
PP
Pierre Picot
LM
Laurent J. Michot
EB
Elodie Barruet
VG
Valérie Geertsen
AT
Antoine Thill
MP
Manuel Pelletier
JB
Jean-Blaise Brubach
PR
Pascale Roy
SC
Sophie Le Caër