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Title: Lanthanide transport in angstrom-scale MoS2-based two-dimensional channels

Journal Article · · Science Advances
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [4]; ORCiD logo [5]; ORCiD logo [2]; ORCiD logo [1]
  1. Univ. of Chicago, IL (United States)
  2. Northwestern Univ., Evanston, IL (United States)
  3. Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
  4. Univ. of Chicago, IL (United States); Jiangxi Normal University, Nanchang (China)
  5. Argonne National Laboratory (ANL), Argonne, IL (United States)

Rare earth elements (REEs), critical to modern industry, are difficult to separate and purify, given their similar physicochemical properties originating from the lanthanide contraction. Here, we systematically study the transport of lanthanide ions (Ln3+) in artificially confined angstrom-scale two-dimensional channels using MoS2-based building blocks in an aqueous environment. The results show that the uptake and permeability of Ln3+ assume a well-defined volcano shape peaked at Sm3+. This transport behavior is rooted from the tradeoff between the barrier for dehydration and the strength of interactions of lanthanide ions in the confinement channels, reminiscent of the Sabatier principle. Molecular dynamics simulations reveal that Sm3+, with moderate hydration free energy and intermediate affinity for channel interaction, exhibit the smallest dehydration degree, consequently resulting in the highest permeability. Our work not only highlights the distinct mass transport properties under extreme confinement but also demonstrates the potential of dialing confinement dimension and chemistry for greener REEs separation.

Research Organization:
Northwestern Univ., Evanston, IL (United States); Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)
Grant/Contract Number:
SC0022231; AC02-06CH11357
OSTI ID:
2339697
Journal Information:
Science Advances, Vol. 10, Issue 11; ISSN 2375-2548
Publisher:
AAASCopyright Statement
Country of Publication:
United States
Language:
English

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Figures / Tables (4)