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Elucidating the Mechanism of a Two-Step Spin Transition in a Nanoporous Metal−Organic Framework
Abstract
The nanoporous metal-organic framework, Fe(bpe)2(NCS)2 x 3(acetone), SCOF-4(Ac) (where bpe is 1,2-bis(4'-pyridyl)ethane), displays a two-step spin crossover (SCO) transition (65-155 K) that is sensitive to the presence of acetone guest molecules. Structural analyses have revealed a structural phase transition, from tetragonal (P42(1)c) to orthorhombic (P2(1)2(1)2), associated with the spin transition that defines a checkerboard-like ordering of spin sites at the high-spin:low-spin plateau. The reversible desorption of the acetone guest species is accompanied by a complex series of structural phase transitions that describe a dramatic flexing of the structure. The thermal trapping of a metastable state with approximately 20-25% high-spin character was observed both magnetically and structurally upon rapid quenching of SCOF-4(Ac) to 10 and 25 K, respectively. The light-induced excited spin state trapping (LIESST) effects for SCOF-4(Ac) show a 55% excitation of a metastable HS state at 10 K and a characteristic T(LIESST) value of 52 K.
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Cited by
Molecular spin crossover phenomenon: recent achievements and prospects
Bousseksou, A., Molnár, G., Salmon, L., & Nicolazzi, W. (2011) · Chemical Society Reviews · doi:10.1039/c1cs15042a · Cited by 1,379
Bloch, E. D., Murray, L. J., Queen, W. L., Chavan, S., Maximoff, S. N., Bigi, J. P., Krishna, R., Peterson, V. K., Grandjean, F., Long, G. J., et al. (2011) · Journal of the American Chemical Society · doi:10.1021/ja205976v · Cited by 531
Recent advances in guest effects on spin-crossover behavior in Hofmann-type metal-organic frameworks
Ni, Z.-P., Liu, J.-L., Hoque, M. N., Liu, W., Li, J.-Y., Chen, Y.-C., & Tong, M.-L. (2017) · Coordination Chemistry Reviews · doi:10.1016/j.ccr.2016.12.002 · Cited by 448
Sumida, K., Horike, S., Kaye, S. S., Herm, Z. R., Queen, W. L., Brown, C. M., Grandjean, F., Long, G. J., Dailly, A., & Long, J. R. (2010) · Chemical Science · doi:10.1039/c0sc00179a · Cited by 347
Entangled Two-Dimensional Coordination Networks: A General Survey
Carlucci, L., Ciani, G., Proserpio, D. M., Mitina, T. G., & Blatov, V. A. (2014) · Chemical Reviews · doi:10.1021/cr500150m · Cited by 285
Metadata
- Authors
- Halder, G. J., Chapman, K. W., Neville, S. M., Moubaraki, B., Murray, K. S., Létard, J.-F., & Kepert, C. J.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2008-12-24
- Volume
- 130
- Issue
- 51
- Pages
- 17552-17562
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2005936801
- Cited by
- 181
- References
- 0
- FWCI
- 4.69
- Type
- journal article
- Language
- en
- Open access
- closed
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- Halder, G. J., Chapman, K. W., Neville, S. M., Moubaraki, B., Murray, K. S., Létard, J.-F., & Kepert, C. J. (2008). Elucidating the Mechanism of a Two-Step Spin Transition in a Nanoporous Metal−Organic Framework. Journal of the American Chemical Society. https://doi.org/10.1021/ja8068038
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