Shedding Light on the Protonation States and Location of Protonated N Atoms of Adenine in Metal-Organic Frameworks.
Shedding Light on the Protonation States and Location of Protonated N Atoms of Adenine in Metal-Organic Frameworks.
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DOI：
10.1021/acs.inorgchem.7b02761
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发表时间：
2018-02-19
影响因子：
4.6
通讯作者：
Stylianou KC
中科院分区：
文献类型：
--
作者：
Gładysiak A;Nguyen TN;Anderson SL;Boyd PG;Palgrave RG;Bacsa J;Smit B;Rosseinsky MJ;Stylianou KC
We report the syntheses and structures of five metal–organic frameworks (MOFs) based on transition metals (NiII, CuII, and ZnII), adenine, and di-, tri-, and tetra-carboxylate ligands. Adenine, with multiple N donor sites, was found to coordinate to the metal centers in different binding modes including bidentate (through N7 and N9, or N3 and N9) and tridentate (through N3, N7, and N9). Systematic investigations of the protonation states of adenine in each MOF structure via X-ray photoelectron spectroscopy revealed that adenine can be selectively protonated through N1, N3, or N7. The positions of H atoms connected to the N atoms were found from the electron density maps, and further supported by the study of C–N–C bond angles compared to the literature reports. DFT calculations were performed to geometrically optimize and energetically assess the structures simulated with different protonation modes. The present study highlights the rich coordination chemistry of adenine and provides a method for the determination of its protonation states and the location of protonated N atoms of adenine within MOFs, a task that would be challenging in complicated adenine-based MOF structures. The protonation states and positions of hydrogen atoms in five adenine-based metal−organic frameworks were revealed using geometrical studies based on single-crystal XRD data supported by XPS spectra and DFT calculations.
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影响因子：
4.6
作者：
Furukawa, Hiroyasu;Go, Yong Bok;Yaghi, Omar M.
通讯作者：
Yaghi, Omar M.
影响因子：
4.6
作者：
Bauer, Sebastian;Serre, Christian;Stock, Norbert
通讯作者：
Stock, Norbert
影响因子：
2.8
作者：
Das, S;Madhavaiah, C;Bharadwaj, PK
通讯作者：
Bharadwaj, PK
影响因子：
3.8
作者：
Burneo, Ivan;Stylianou, Kyriakos C.;Maspoch, Daniel
通讯作者：
Maspoch, Daniel
DOI：
10.1107/s2052520616003954
发表时间：
2016-04
期刊：
Acta crystallographica Section B, Structural science, crystal engineering and materials
影响因子：
--
作者：
Groom CR;Bruno IJ;Lightfoot MP;Ward SC
通讯作者：
Ward SC