| 研究実績の概要 |
First, we have performed systematic high-level DFT cluster calculations mimicking modified IRMOF materials at the B3LYP/6-31G* level. The resulting structures are obtained by replacement of beryllium-based metal-oxide connector parts with more complex magnesium-titanium oxide parts leading to an increased unit-cell volume size as well as the basicity of oxide centres of whole structures that makes one effectively tune active sites for hydrogen activation and storage. The overall cluster thus obtained has the C160H96Mg4O96Ti12 stoichiometry. Using a part of this extended cluster model of C48H32MgO28Ti3 and two-layer ONIOM(MP2/6-31G*:HF/3-21G) approach, we have estimated the binding energy of molecular hydrogen to be 1.29 kcal/mol which is twice as large as the value for similar non-modified beryllium-based precursor one. Both the increased unit-cell size and more basic oxide sites of thus modified IRMOF structure makes it as efficient and potential material for hydrogen storage and related other applications.
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