Structural disorder and transformation in crystal growth: direct observation of ring-opening isomerization in a metal–organic solid solution
A rare example is reported in which discrete Ag2L2 ring and (AgL)∞ chain motifs [L = N,N′-bis(3-imidazol-1-yl-propyl)-pyromellitic diimide] co-crystallize in the same crystal lattice with varying ratios and degrees of disorder. Crystal structures obtained from representative crystals reveal compatib...
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| Format: | Article |
| Language: | English |
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International Union of Crystallography
2014-09-01
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| Series: | IUCrJ |
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| Online Access: | http://scripts.iucr.org/cgi-bin/paper?S2052252514015966 |
| _version_ | 1819281710516273152 |
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| author | Ji-Jun Jiang Jian-Rong He Xing-Qiang Lü Da-Wei Wang Guo-Bi Li Cheng-Yong Su |
| author_facet | Ji-Jun Jiang Jian-Rong He Xing-Qiang Lü Da-Wei Wang Guo-Bi Li Cheng-Yong Su |
| author_sort | Ji-Jun Jiang |
| collection | DOAJ |
| description | A rare example is reported in which discrete Ag2L2 ring and (AgL)∞ chain motifs [L = N,N′-bis(3-imidazol-1-yl-propyl)-pyromellitic diimide] co-crystallize in the same crystal lattice with varying ratios and degrees of disorder. Crystal structures obtained from representative crystals reveal compatible packing arrangements of the cyclic and polymeric isomers within the crystal lattice, which enables them to co-exist within a crystalline solid solution. A feasible pathway for transformation between the isomers is suggested via facile rotation of the coordinating imidazolyl groups. This chemical system could provide a chance for direct observation of ring-opening isomerization at the crystal surface. Mass spectrometry and 1H NMR titration show a dynamic equilibrium between cyclic and oligomeric species in solution, and a potential crystallization process is suggested involving alignment of precursors directed by aromatic stacking interactions between pyromellitic diimide units, followed by ring-opening isomerization at the interface between the solid and the solution. Both cyclic and oligomeric species can act as precursors, with interconversion between them being facile due to a low energy barrier for rotation of the imidazole rings. Thermogravimetric analysis and variable-temperature powder X-ray diffraction indicate a transition to a different crystalline phase around 120°C, which is associated with loss of solvent from the crystal lattice. |
| first_indexed | 2024-12-24T01:04:01Z |
| format | Article |
| id | doaj.art-59ff1e999b674866833ce3acd915d419 |
| institution | Directory Open Access Journal |
| issn | 2052-2525 |
| language | English |
| last_indexed | 2024-12-24T01:04:01Z |
| publishDate | 2014-09-01 |
| publisher | International Union of Crystallography |
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| series | IUCrJ |
| spelling | doaj.art-59ff1e999b674866833ce3acd915d4192022-12-21T17:23:17ZengInternational Union of CrystallographyIUCrJ2052-25252014-09-011531832710.1107/S2052252514015966bi5033Structural disorder and transformation in crystal growth: direct observation of ring-opening isomerization in a metal–organic solid solutionJi-Jun Jiang0Jian-Rong He1Xing-Qiang Lü2Da-Wei Wang3Guo-Bi Li4Cheng-Yong Su5MOE Laboratory of Bioinorganic and Synthetic Chemistry, State Key Laboratory of Optoelectronic Materials and Technologies, Lehn Institute of Functional Materials, School of Chemistry and Chemical Engineering, Sun Yet-Sun University, Guangzhou 510275, People's Republic of ChinaMOE Laboratory of Bioinorganic and Synthetic Chemistry, State Key Laboratory of Optoelectronic Materials and Technologies, Lehn Institute of Functional Materials, School of Chemistry and Chemical Engineering, Sun Yet-Sun University, Guangzhou 510275, People's Republic of ChinaMOE Laboratory of Bioinorganic and Synthetic Chemistry, State Key Laboratory of Optoelectronic Materials and Technologies, Lehn Institute of Functional Materials, School of Chemistry and Chemical Engineering, Sun Yet-Sun University, Guangzhou 510275, People's Republic of ChinaMOE Laboratory of Bioinorganic and Synthetic Chemistry, State Key Laboratory of Optoelectronic Materials and Technologies, Lehn Institute of Functional Materials, School of Chemistry and Chemical Engineering, Sun Yet-Sun University, Guangzhou 510275, People's Republic of ChinaMOE Laboratory of Bioinorganic and Synthetic Chemistry, State Key Laboratory of Optoelectronic Materials and Technologies, Lehn Institute of Functional Materials, School of Chemistry and Chemical Engineering, Sun Yet-Sun University, Guangzhou 510275, People's Republic of ChinaMOE Laboratory of Bioinorganic and Synthetic Chemistry, State Key Laboratory of Optoelectronic Materials and Technologies, Lehn Institute of Functional Materials, School of Chemistry and Chemical Engineering, Sun Yet-Sun University, Guangzhou 510275, People's Republic of ChinaA rare example is reported in which discrete Ag2L2 ring and (AgL)∞ chain motifs [L = N,N′-bis(3-imidazol-1-yl-propyl)-pyromellitic diimide] co-crystallize in the same crystal lattice with varying ratios and degrees of disorder. Crystal structures obtained from representative crystals reveal compatible packing arrangements of the cyclic and polymeric isomers within the crystal lattice, which enables them to co-exist within a crystalline solid solution. A feasible pathway for transformation between the isomers is suggested via facile rotation of the coordinating imidazolyl groups. This chemical system could provide a chance for direct observation of ring-opening isomerization at the crystal surface. Mass spectrometry and 1H NMR titration show a dynamic equilibrium between cyclic and oligomeric species in solution, and a potential crystallization process is suggested involving alignment of precursors directed by aromatic stacking interactions between pyromellitic diimide units, followed by ring-opening isomerization at the interface between the solid and the solution. Both cyclic and oligomeric species can act as precursors, with interconversion between them being facile due to a low energy barrier for rotation of the imidazole rings. Thermogravimetric analysis and variable-temperature powder X-ray diffraction indicate a transition to a different crystalline phase around 120°C, which is associated with loss of solvent from the crystal lattice.http://scripts.iucr.org/cgi-bin/paper?S2052252514015966crystallizationstructural transformationring-opening isomerismsolid solutiondisorder |
| spellingShingle | Ji-Jun Jiang Jian-Rong He Xing-Qiang Lü Da-Wei Wang Guo-Bi Li Cheng-Yong Su Structural disorder and transformation in crystal growth: direct observation of ring-opening isomerization in a metal–organic solid solution IUCrJ crystallization structural transformation ring-opening isomerism solid solution disorder |
| title | Structural disorder and transformation in crystal growth: direct observation of ring-opening isomerization in a metal–organic solid solution |
| title_full | Structural disorder and transformation in crystal growth: direct observation of ring-opening isomerization in a metal–organic solid solution |
| title_fullStr | Structural disorder and transformation in crystal growth: direct observation of ring-opening isomerization in a metal–organic solid solution |
| title_full_unstemmed | Structural disorder and transformation in crystal growth: direct observation of ring-opening isomerization in a metal–organic solid solution |
| title_short | Structural disorder and transformation in crystal growth: direct observation of ring-opening isomerization in a metal–organic solid solution |
| title_sort | structural disorder and transformation in crystal growth direct observation of ring opening isomerization in a metal organic solid solution |
| topic | crystallization structural transformation ring-opening isomerism solid solution disorder |
| url | http://scripts.iucr.org/cgi-bin/paper?S2052252514015966 |
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