Journal
ADVANCED MATERIALS INTERFACES
Volume 9, Issue 31, Pages -Publisher
WILEY
DOI: 10.1002/admi.202201484
Keywords
anions; charge distribution control; layered double hydroxide; low nucleophilicity; on-target separation
Funding
- Environment Research and Technology Development Fund [5RF-1902]
- Environmental Restoration and Conservation Agency of Japan
- JSPS KAKENHI [22H00568, 22H04533, 21K14404, 20H05214]
- MEXT Program for Building Regional Innovation Ecosystem
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This study demonstrates that guest-guest interactions significantly influence the separation of low nucleophilicity nitrate using layered double hydroxides (LDHs). By applying a topochemical reaction to control the cation arrangement in LDHs, a hexagonal cation arrangement is facilitated, leading to improved ion storage capacity and effective separation.
Host-guest chemistry principles and mechanisms have been exploited to separate harmful and valuable ionic species. However, separating low nucleophilicity anions using these protocols is difficult due to weak host-guest interactions. Herein, using layered double hydroxides (LDHs), it is demonstrated that guest-guest interactions considerably influence the separation of a low nucleophilicity nitrate. LDHs exhibit considerably low nitrate ion storage capacities due to the co-precipitation synthesis method. Hence, a topochemical reaction is applied to control the cation arrangement in the LDHs. Structural analyses determine that a hexagonal cation arrangement is facilitated. Isotherm analysis reveals that the obtained LDHs improve the capacity up to 250% of that of typical less-ordered LDHs. Finally, further isotherm analysis in combination with theoretical calculations, it is revealed that the hexagonal arrangement effectively facilitates a stable guest-guest interactions-hydrogen-bond between the interlayer nitrate ions and water molecules, which contributes to high ion-storage.
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