Title: Tailored Synthesis of the Narrowest Zigzag Graphene Nanoribbon Structure by Compressing the Lithium Acetylide under High Temperature

Abstract

Scientists are searching for the goal-directed methods to synthesize graphene nanoribbons (GNRs) with a particular edge type and width, which determines their electronic transport properties. A series of Li zigzag GNRs (ZGNRs) with different widths were predicted under high pressure with a stoichiometric ratio of Li_n+1C_2n, which indicates a route to prepare ultranarrow GNRs. Here, with thermodynamics and ab initio Gibbs free-energy calculations by quasi-harmonic approximation, we investigated the phase stabilities of the Li GNR compounds under high pressure and high temperature. We have also identified Li graphenide LiC₂ (n = ∞) and Li polyacenide Li₃C₄ (n = 2) experimentally at the predicted pressure and temperature conditions using in situ X-ray diffraction, which can be recognized as the two end members of Li_n+1C_2n, with the widest and narrowest ZGNR structures. High temperature and the temperature gradient increased the degree of polymerization and facilitated the formation of wider GNR or carbon slices. Furthermore, this suggests that by controlling temperature and pressure, we may get ultranarrow Li ZGNRs composed of a limited number of parallel carbon chains, such as 3- or 4-zigzag GNR, which is ready to be protonated or functionalized to form atomically ordered ZGNRs.

Authors:

Dong, Xiao ^[1]; Wang, Lijuan ^[1]; Li, Kuo  ^[1];

• Search DOE PAGES for author "Li, Kuo"
• Search DOE PAGES for ORCID "0000-0002-4859-6099"

Zheng, Haiyan  ^[1];

• Search DOE PAGES for author "Zheng, Haiyan"
• Search DOE PAGES for ORCID "0000-0002-4727-5912"

Wang, Yajie ^[1]; Meng, Yue ^[2]; Shu, Haiyun ^[1]; Mao, Ho-kwang ^[3]; Feng, Shaomin ^[4]; Jin, Changqing ^[4]

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+ Show Author Affiliations

1. Center for High Pressure Science and Technology Advanced Research, Beijing (China)
2. Argonne National Lab. (ANL), Argonne, IL (United States)
3. Center for High Pressure Science and Technology Advanced Research, Beijing (China); Carnegie Institution of Washington, Washington, D.C. (United States)
4. Chinese Academy of Sciences (CAS), Beijing (China); Collaborative Innovation Centre of Quantum Matter, Beijing (China)

Publication Date:

Mon Aug 13 00:00:00 EDT 2018

Research Org.:

Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE National Nuclear Security Administration (NNSA)

OSTI Identifier:

1484369

Grant/Contract Number:  

AC02-06CH11357

Resource Type:

Accepted Manuscript

Journal Name:

Journal of Physical Chemistry. C

Additional Journal Information:

Journal Volume: 122; Journal Issue: 35; Journal ID: ISSN 1932-7447

Publisher:

American Chemical Society

Country of Publication:

United States

Language:

English

Subject:

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY