Abstract:Separation of actinides from lanthanides is of great importance for the safe management of nuclear waste and sustainable development of nuclear energy, but it represents a huge challenge due to the chemical complexity of these f-elements. Herein, we report an efficient separation strategy based on ion sieving in graphene oxide membrane. In the presence of a strong oxidizing reagent, the actinides (U, Np, Pu, Am) in a nitric acid solution exist in the high valent and linear dioxo form of actinyl ions while the … Show more
“…Indeed, works have demonstrated impressive ion separations using GO membranes. 110,111 Another work demonstrated three-dimensional GO structures with impressive ion sorptions. 112 However, little information has been provided about the exact interactions between the GO flakes, adsorbed ions, flowing liquid water, and interlayer supports.…”
Section: Ion Adsorption and Water Behaviour In Three-dimensional Grap...mentioning
Understanding molecular-scale information about water and ion interactions at graphene and graphene oxide surfaces is critical for successful application development.
“…Indeed, works have demonstrated impressive ion separations using GO membranes. 110,111 Another work demonstrated three-dimensional GO structures with impressive ion sorptions. 112 However, little information has been provided about the exact interactions between the GO flakes, adsorbed ions, flowing liquid water, and interlayer supports.…”
Section: Ion Adsorption and Water Behaviour In Three-dimensional Grap...mentioning
Understanding molecular-scale information about water and ion interactions at graphene and graphene oxide surfaces is critical for successful application development.
“…The prepared G/Z/M membrane was used to separate the Li + , Na + , K + , and Mg 2+ ion mixture solution, and the samples were analyzed by inductively coupled plasma optical emission spectroscopy (ICP-OES) for the concentration of each ion and the permeation percentages (Pct) was calculated using the following equation Pct=CtC0 where C t is the measured concentration of the metal ion in ppm and C 0 is the concentration of the starting ion of the permeate.…”
Selective ion separation
from brines is pivotal for attaining
high-purity
lithium, a critical nonrenewable resource. Conventional methods encounter
substantial challenges, driving the quest for streamlined, efficient,
and swift approaches. Here, we present a graphene oxide (GO)-based
ternary heterostructure membrane with a unique design. By utilizing
Zn2+-induced confinement synthesis in a two-dimensional
(2D) space, we incorporated two-dimensional zeolitic imidazolate framework-8
(ZIF-8) and zinc alginate (ZA) polymers precisely within layers of
the GO membrane, creating tunable interlayer channels with a ternary
heterostructure. The pivotal design lies in ion insertion into the
two-dimensional (2D) membrane layers, achieving meticulous modulation
of layer spacing based on ion hydration radius. Notably, the ensuing
layer spacing within the hybrid ionic intercalation membrane occupies
an intermediary realm, positioned astutely between small-sized hydrated
ionic intercalation membrane spacing and their more extensive counterparts.
This deliberate configuration accelerates the swift passage of diminutive
hydrated ions while simultaneously impeding the movement of bulkier
ions within the brine medium. The outcome is remarkable selectivity,
demonstrated by the partitioning of K+/Li+ =
20.9, Na+/K+ = 31.2, and Li+/Mg2+ = 9.5 ion pairs. The ZIF-8/GO heterostructure significantly
contributes to the selectivity, while the mechanical robustness and
stability, improved by the ZA/GO heterostructure, further support
its practical applicability. This report reports an advanced membrane
design, offering promising prospects for lithium extraction and various
ion separation processes.
“…After a period of time, the nuclear fuel must be replaced, and the resulting waste is known as spent (or old) nuclear fuel (SNF). It still contains 95% uranium, which can be recycled to improve the utilization rate of uranium resources. − …”
During
the PUREX process, the separation between U(VI)
and Pu(IV)
is achieved by reducing Pu(IV) to Pu(III), which is complicated and
energy-consuming. To address this issue, we report here the first
case of separation of U(VI) from Pu(IV) by o-phenanthroline
diamide ligands under high acidity. Two new o-phenanthroline
diamide ligands (1,10-phenanthroline-2,9-diyl)bis(indolin-1-ylmethanone)
(L1) and (1,10-phenanthroline-2,9-diyl)bis((2-methylindolin-1-yl)methanone)
(L2) were synthesized, which can effectively separate U(VI) from Pu(IV)
even at 4 mol/L HNO3. The highest separation factor of
U(VI) and Pu(IV) can reach over 1000, setting a new record for the
separation of U(VI) from Pu(IV) under high acidity. Furthermore,
extracted U(VI) can be easily recovered with water or dilute nitric
acid, and the extraction performance remains stable even after 150
kGy gamma irradiation, which provides solid experimental support for
potential engineering applications. The results of UV–vis titration
and single-crystal X-ray diffraction measurements show that the 1:1
complex formed by L1 with U(VI) is more stable than all of the previously
reported phenanthroline ligands, which reasonably reveals that the
ligand L1 designed in this work has excellent affinity for U(VI).
The findings of this work promise to contribute to the facilitation
of the PUREX process by avoiding the use of reducing agents. It also
provides new clues for designing ligands to achieve efficient separation
between U(VI) and Pu(IV) at high acidity.
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