Journal
NATURE COMMUNICATIONS
Volume 13, Issue 1, Pages -Publisher
NATURE PORTFOLIO
DOI: 10.1038/s41467-022-35386-z
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Funding
- National Research Foundation of Korea (NRF) - Ministry of Education [NRF-2020R1A2C4001617, NRF-2021M3H4A1A02055684]
- Air Environment Complex Response programs [2E31663, 2E31711]
- Korea Institute of Science and Technology (KIST)
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This study demonstrates precise multiscale structural control of chalcogenide aerogels through self-assembly of thiostannate motifs. The aerogels showed varying specific surface areas, coordination networks, crystallinity, and porous structures. They also successfully adopted the structure and ion-exchange principles of two-dimensional metal sulfides.
Chalcogenide aerogels (chalcogels) are amorphous structures widely known for their lack of localized structural control. This study, however, demonstrates a precise multiscale structural control through a thiostannate motif ([Sn2S6](4-))-transformation-induced self-assembly, yielding Na-Mn-Sn-S, Na-Mg-Sn-S, and Na-Sn(II)-Sn(IV)-S aerogels. The aerogels exhibited [Sn2S6](4-):Mn2+ stoichiometric-variation-induced-control of average specific surface areas (95-226 m(2) g(-1)), thiostannate coordination networks (octahedral to tetrahedral), phase crystallinity (crystalline to amorphous), and hierarchical porous structures (micropore-intensive to mixed-pore state). In addition, these chalcogels successfully adopted the structural motifs and ion-exchange principles of two-dimensional layered metal sulfides (K2xMnxSn3-xS6, KMS-1), featuring a layer-by-layer stacking structure and effective radionuclide (Cs+, Sr2+)-control functionality. The thiostannate cluster-based gelation principle can be extended to afford Na-Mg-Sn-S and Na-Sn(II)-Sn(IV)-S chalcogels with the same structural features as the Na-Mn-Sn-S chalcogels (NMSCs). The study of NMSCs and their chalcogel family proves that the self-assembly principle of two-dimensional chalcogenide clusters can be used to design unique chalcogels with unprecedented structural hierarchy.
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