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Light-Harvesting and Ultrafast Energy Migration in Porphyrin-Based Metal–Organic Frameworks
Abstract
Given that energy (exciton) migration in natural photosynthesis primarily occurs in highly ordered porphyrin-like pigments (chlorophylls), equally highly ordered porphyrin-based metal-organic frameworks (MOFs) might be expected to exhibit similar behavior, thereby facilitating antenna-like light-harvesting and positioning such materials for use in solar energy conversion schemes. Herein, we report the first example of directional, long-distance energy migration within a MOF. Two MOFs, namely F-MOF and DA-MOF that are composed of two Zn(II) porphyrin struts [5,15-dipyridyl-10,20-bis(pentafluorophenyl)porphinato]zinc(II) and [5,15-bis[4-(pyridyl)ethynyl]-10,20-diphenylporphinato]zinc(II), respectively, were investigated. From fluorescence quenching experiments and theoretical calculations, we find that the photogenerated exciton migrates over a net distance of up to ~45 porphyrin struts within its lifetime in DA-MOF (but only ~3 in F-MOF), with a high anisotropy along a specific direction. The remarkably efficient exciton migration in DA-MOF is attributed to enhanced π-conjugation through the addition of two acetylene moieties in the porphyrin molecule, which leads to greater Q-band absorption intensity and much faster exciton-hopping (energy transfer between adjacent porphyrin struts). The long distance and directional energy migration in DA-MOF suggests promising applications of this compound or related compounds in solar energy conversion schemes as an efficient light-harvesting and energy-transport component.
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Lessons from nature about solar light harvesting
Scholes, G. D., Fleming, G. R., Olaya-Castro, A., & van Grondelle, R. (2011) · Nature Chemistry · doi:10.1038/nchem.1145 · Cited by 1,915
Large-scale screening of hypothetical metal–organic frameworks
Wilmer, C. E., Leaf, M., Lee, C. Y., Farha, O. K., Hauser, B. G., Hupp, J. T., & Snurr, R. Q. (2012) · Nature Chemistry · doi:10.1038/nchem.1192 · Cited by 1,439
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Cited by
Metal–organic frameworks as platforms for clean energy
Li, S.-L., & Xu, Q. (2013) · Energy & Environmental Science · doi:10.1039/c3ee40507a · Cited by 970
Ding, Y., Chen, Y.-P., Zhang, X., Chen, L., Dong, Z., Jiang, H.-L., Xu, H., & Zhou, H.-C. (2017) · Journal of the American Chemical Society · doi:10.1021/jacs.7b04829 · Cited by 470
Pore Chemistry of Metal–Organic Frameworks
Ji, Z., Wang, H., Canossa, S., Wuttke, S., & Yaghi, O. M. (2020) · Advanced Functional Materials · doi:10.1002/adfm.202000238 · Cited by 459
Activation of metal–organic framework materials
Mondloch, J. E., Karagiaridi, O., Farha, O. K., & Hupp, J. T. (2013) · CrystEngComm · doi:10.1039/c3ce41232f · Cited by 324
Self-citationGiant light-harvesting nanoantenna for single-molecule detection in ambient light
Trofymchuk, K., Reisch, A., Didier, P., Fras, F., Gilliot, P., Mely, Y., & Klymchenko, A. S. (2017) · Nature Photonics · doi:10.1038/s41566-017-0001-7 · Cited by 175
Metadata
- Authors
- Son, H.-J., Jin, S., Patwardhan, S., Wezenberg, S. J., Jeong, N. C., So, M., Wilmer, C. E., Sarjeant, A. A., Schatz, G. C., Snurr, R. Q., Farha, O. K., Wiederrecht, G. P., & Hupp, J. T.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2013-01-02
- Volume
- 135
- Issue
- 2
- Pages
- 862-869
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2056896873
- Cited by
- 592
- References
- 2
- FWCI
- 21.72
- Type
- journal article
- Language
- en
- Open access
- closed
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- Son, H.-J., Jin, S., Patwardhan, S., Wezenberg, S. J., Jeong, N. C., So, M., Wilmer, C. E., Sarjeant, A. A., Schatz, G. C., Snurr, R. Q., Farha, O. K., Wiederrecht, G. P., & Hupp, J. T. (2013). Light-Harvesting and Ultrafast Energy Migration in Porphyrin-Based Metal–Organic Frameworks. Journal of the American Chemical Society. https://doi.org/10.1021/ja310596a
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