Carbon-based nanomaterials have exceptional properties that make them attractive for a variety of technological applications. Here, we report on the use of diamondoids (diamond-like, saturated hydrocarbons) as promising precursors for laser-induced high-pressure, high-temperature diamond synthesis. The lowest pressure and temperature (P-T) conditions that yielded diamond were 12 GPa (at ~2000 K) and 900 K (at ~20 GPa), respectively. This represents a substantially reduced transformation barrier compared with diamond synthesis from conventional (hydro)carbon allotropes, owing to the similarities in the structure and full sp3hybridization of diamondoids and bulk diamond. At 20 GPa, diamondoid-to-diamond conversion occurs rapidly within <19 μs. Molecular dynamics simulations indicate that once dehydrogenated, the remaining diamondoid carbon cages reconstruct themselves into diamond-like structures at high P-T. This study is the first successful mapping of the P-T conditions and onset timing of the diamondoid-to-diamond conversion and elucidates the physical and chemical factors that facilitate diamond synthesis.
Park, Sulgiye, Abate, Iwnetim I., Liu, Jin, Wang, Chenxu, Dahl, Jeremy E. P., Carlson, Robert M. K., Yang, Liuxiang, Prakapenka, Vitali B., Greenberg, Eran, Devereaux, Thomas P., Jia, Chunjing, Ewing, Rodney C., Mao, Wendy L., & Lin, Yu (2020). Facile diamond synthesis from lower diamondoids. Science Advances, 6(8). https://doi.org/10.1126/sciadv.aay9405
@article{osti_1601857,
author = {Park, Sulgiye and Abate, Iwnetim I. and Liu, Jin and Wang, Chenxu and Dahl, Jeremy E. P. and Carlson, Robert M. K. and Yang, Liuxiang and Prakapenka, Vitali B. and Greenberg, Eran and Devereaux, Thomas P. and others},
title = {Facile diamond synthesis from lower diamondoids},
annote = {Carbon-based nanomaterials have exceptional properties that make them attractive for a variety of technological applications. Here, we report on the use of diamondoids (diamond-like, saturated hydrocarbons) as promising precursors for laser-induced high-pressure, high-temperature diamond synthesis. The lowest pressure and temperature (P-T) conditions that yielded diamond were 12 GPa (at ~2000 K) and 900 K (at ~20 GPa), respectively. This represents a substantially reduced transformation barrier compared with diamond synthesis from conventional (hydro)carbon allotropes, owing to the similarities in the structure and full sp3hybridization of diamondoids and bulk diamond. At 20 GPa, diamondoid-to-diamond conversion occurs rapidly within P-T. This study is the first successful mapping of the P-T conditions and onset timing of the diamondoid-to-diamond conversion and elucidates the physical and chemical factors that facilitate diamond synthesis.},
doi = {10.1126/sciadv.aay9405},
url = {https://www.osti.gov/biblio/1601857},
journal = {Science Advances},
issn = {ISSN 2375-2548},
number = {8},
volume = {6},
place = {United States},
publisher = {AAAS},
year = {2020},
month = {02}}
Philosophical Transactions of the Royal Society of London. Series A: Mathematical, Physical and Engineering Sciences, Vol. 362, Issue 1824https://doi.org/10.1098/rsta.2004.1454