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Title: Facile diamond synthesis from lower diamondoids

Abstract

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.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2];  [3];  [4];  [4];  [5]; ORCiD logo [6]; ORCiD logo [7]; ORCiD logo [1]; ORCiD logo [4];  [3];  [1]; ORCiD logo [4]
  1. Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)
  2. Stanford Univ., CA (United States); Center for High Pressure Science and Technology Advanced Research, Beijing (China)
  3. Stanford Univ., CA (United States)
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)
  5. Center for High Pressure Science and Technology Advanced Research, Beijing (China)
  6. Univ. of Chicago, IL (United States). Center for Advanced Radiation Sources (CARS)
  7. Univ. of Chicago, IL (United States). Center for Advanced Radiation Sources (CARS); Soreq Nuclear Research Center, Yavne (Israel)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1574721
Grant/Contract Number:  
AC02-76SF00515; FG02-94ER14466; EAR-1634415; AC02-06CH11357; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Science Advances
Additional Journal Information:
Journal Volume: 6; Journal Issue: 8; Journal ID: ISSN 2375-2548
Publisher:
AAAS
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

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., and Lin, Yu. Facile diamond synthesis from lower diamondoids. United States: N. p., 2020. Web. doi:10.1126/sciadv.aay9405.
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. Facile diamond synthesis from lower diamondoids. United States. https://doi.org/10.1126/sciadv.aay9405
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., and Lin, Yu. Fri . "Facile diamond synthesis from lower diamondoids". United States. https://doi.org/10.1126/sciadv.aay9405. https://www.osti.gov/servlets/purl/1574721.
@article{osti_1574721,
title = {Facile diamond synthesis from lower diamondoids},
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 Jia, Chunjing and Ewing, Rodney C. and Mao, Wendy L. and Lin, Yu},
abstractNote = {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.},
doi = {10.1126/sciadv.aay9405},
journal = {Science Advances},
number = 8,
volume = 6,
place = {United States},
year = {2020},
month = {2}
}

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