2020 Fiscal Year Research-status Report
Compartmentalization of catalysts into metal-organic polyhedra gel for cascade reactions
| Project/Area Number |
20K15366
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| Research Institution | Kyoto University |
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Principal Investigator |
LEGRAND ALEX 京都大学, 高等研究院, 特定研究員 (00836372)
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| Project Period (FY) |
2020-04-01 – 2022-03-31
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| Keywords | metal-organic polyhedra / self-assembly / soft matter / catalysis / metal nanoparticle |
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| Outline of Annual Research Achievements |
OHRhMOP and C12RhMOP have been synthesized. 2 strategies were used to isolate metal nanoparticles (MNP) within the cage. The first one involves the direct mixing of metal precursor with OHRhMOP in MeOH but didn’t led to incorporation of the MNP as demonstrated by DLS, TEM and PXRD analysis. In contrast, the 2nd strategy, which requires the phase transfer of the metal ion from an aqueous solution to an organic one containing the C12RhMOP and its reduction, leaded to promising results. DLS, TEM and PXRD demonstrated the potential presence of particle with a size of ~1.3 nm within the cage. Control experiment showed that without the cage, the same reaction lead to the formation of aggregated particle of ~ 247 nm. Similar results were obtained when using Pd instead of Au metal precursor.
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| Current Status of Research Progress |
Current Status of Research Progress
2: Research has progressed on the whole more than it was originally planned.
Reason
It remains difficult to assess for the presence of the MNPs within the cage. In addition, it was not possible so far to process the MNPs@MOP solution into the gel as previously reported by our group with the pristine MOP. This is due to the different solvent used for the encapsulation of the MNP (DCM) and the supramolecular polymerization reaction leading to the soft matter (DMF). Strategy to replace the DCM after MNPS synthesis with DMF have been envisaged and need to be optimized.
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| Strategy for Future Research Activity |
Direct evidence of the encapsulation of the MNP within the cage is still necessary. Optimization of the synthesis and washing protocol is ongoing. In addition, recrystallization of the cage in order to obtain single crystal is in progress. This could give direct evidence, once the structure is resolved by SCXRD, of the localization of the MNPs.
A 3rd strategy will be investigated, which require the addition of few uL of an aqueous solution of the metal precursor in a hydrophobic solution (DCM) of the C12RhMOP cage, which has hydrophilic cavity.
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| Causes of Carryover |
In reason of COVID situation, no budget have been use to travel for collaboration or international conferences
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