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Dinitrogen Dissociation on an Isolated Surface Tantalum Atom
Open accessAbstract
Both industrial and biochemical ammonia syntheses are thought to rely on the cooperation of multiple metals in breaking the strong triple bond of dinitrogen. Such multimetallic cooperation for dinitrogen cleavage is also the general rule for dinitrogen reductive cleavage with molecular systems and surfaces. We have observed cleavage of dinitrogen at 250°C and atmospheric pressure by dihydrogen on isolated silica surface–supported tantalum(III) and tantalum(V) hydride centers [(≡Si-O) 2 Ta III -H] and [(≡Si-O) 2 Ta V H 3 ], leading to the Ta V amido imido product [(≡SiO) 2 Ta(=NH)(NH 2 )]: We assigned the product structure based on extensive characterization by infrared and solid-state nuclear magnetic resonance spectroscopy, isotopic labeling studies, and supporting data from x-ray absorption and theoretical simulations. Reaction intermediates revealed by in situ monitoring of the reaction with infrared spectroscopy support a mechanism highly distinct from those previously observed in enzymatic, organometallic, and heterogeneous N 2 activating systems.
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Citations
Cited by
Wang, P., Chang, F., Gao, W., Guo, J., Wu, G., He, T., & Chen, P. (2017) · Nature Chemistry · doi:10.1038/nchem.2595 · Cited by 711
Surface Enhanced NMR Spectroscopy by Dynamic Nuclear Polarization
Lesage, A., Lelli, M., Gajan, D., Caporini, M. A., Vitzthum, V., Miéville, P., Alauzun, J., Roussey, A., Thieuleux, C., Mehdi, A., et al. (2010) · Journal of the American Chemical Society · doi:10.1021/ja104771z · Cited by 585
Self-citationTitanium-Based Hydrides as Heterogeneous Catalysts for Ammonia Synthesis
Kobayashi, Y., Tang, Y., Kageyama, T., Yamashita, H., Masuda, N., Hosokawa, S., & Kageyama, H. (2017) · Journal of the American Chemical Society · doi:10.1021/jacs.7b08891 · Cited by 282
Fresh perspectives for surface coordination chemistry
Barth, J. V. (2009) · Surface Science · doi:10.1016/j.susc.2008.09.049 · Cited by 261
Mao, C., Li, H., Gu, H., Wang, J., Zou, Y., Qi, G., Xu, J., Deng, F., Shen, W., Li, J., et al. (2019) · Chem · doi:10.1016/j.chempr.2019.07.021 · Cited by 180
Metadata
- Authors
- Avenier, P., Taoufik, M., Lesage, A., Solans-Monfort, X., Baudouin, A., de Mallmann, A., Veyre, L., Basset, J.-M., Eisenstein, O., Emsley, L., & Quadrelli, E. A.
- Venue
- Science
- Published
- 2007-08-24
- Volume
- 317
- Issue
- 5841
- Pages
- 1056-1060
- ISSN
- 0036-8075 (ISSN-L)
- 1095-9203
- OpenAlex
- W2035417009
- Cited by
- 187
- References
- 0
- FWCI
- 5.03
- Type
- journal article
- Language
- en
- Open access
- green
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- Avenier, P., Taoufik, M., Lesage, A., Solans-Monfort, X., Baudouin, A., de Mallmann, A., Veyre, L., Basset, J.-M., Eisenstein, O., Emsley, L., & Quadrelli, E. A. (2007). Dinitrogen Dissociation on an Isolated Surface Tantalum Atom. Science. https://doi.org/10.1126/science.1143078
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