137
Cs
with strong radioactivity and a long half-life
is highly hazardous to human health and the environment. The efficient
removal of
137
Cs from complex solutions is still challenging
because of its high solubility and easy mobility and the influence
of interfering ions. It is highly desirable to develop effective scavengers
for radiocesium remediation. Here, the highly efficient uptake of
Cs
+
has been realized by two robust layered metal–organic
frameworks (MOFs), namely [(CH
3
)
2
NH
2
]In(L)
2
·DMF·H
2
O (DMF =
N
,
N
′-dimethylformamide, H
2
L= H
2
aip (5-aminoisophthalic acid) for
1
and H
2
hip (5-hydroxyisophthalic acid) for
2
). Remarkably,
1
and
2
hold excellent acid and alkali resistance
and radiation stabilities. They exhibit fast kinetics, high capacities
(
q
m
Cs
= 270.86 and 297.67 mg/g for
1
and
2
, respectively), excellent selectivity for Cs
+
uptake,
and facile elution for the regeneration of materials. Particularly,
1
and
2
can achieve efficient Cs
+
/Sr
2+
separation in a wide range of Sr/Cs molar ratios. For example,
the separation factor (
SF
Cs/Sr
) is up
to ∼320 for
1
. Moreover, the Cs
+
uptake
and elution mechanisms have been directly elucidated at the molecular
level by an unprecedented single-crystal to single-crystal (SC-SC)
structural transformation, which is attributed to the strong interactions
between COO
–
functional groups and Cs
+
ions, easily exchangeable [(CH
3
)
2
NH
2
]
+
, and flexible and robust anionic layer frameworks with
open windows as “pockets”. This work highlights layered
MOFs for the highly efficient uptake of Cs
+
ions in the
field of radionuclide remediation.