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Graphitization of low-density amorphous carbon for electrocatalysis electrodes from ReaxFF reactive dynamics

Hossain, Md Delowar and Zhang, Qing and Cheng, Tao and Goddard, William A., III and Luo, Zhengtang (2021) Graphitization of low-density amorphous carbon for electrocatalysis electrodes from ReaxFF reactive dynamics. Carbon, 183 . pp. 940-947. ISSN 0008-6223. doi:10.1016/j.carbon.2021.07.080. https://resolver.caltech.edu/CaltechAUTHORS:20210823-204347903

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Abstract

We predict the three-dimensional structure of amorphous carbon generated by heating diamond superlattice at 6000 K with rapid quenching from the liquid phase for densities ranging from 2.0 to 3.5 g/cm³, in comparison with 2.26 and 3.54 g/cm³ for bulk graphite and bulk diamond, respectively. These predictions are based on reactive dynamics (RD) simulations using the ReaxFF reactive force field. Here, we simulate the graphitization of amorphous carbon at high temperature to calculate physical properties relevant to conductive carbon supports useful for electrocatalysts. The low-density graphitic materials mostly oriented in the (002) plane with a main X-ray diffraction (XRD) peak between 26 and 28°, as observed experimentally. For low density carbon (2.0–2.5 g/cm³), we find >90% sp² character with ∼2-1% sp and <8% sp³. While for higher density carbon, the amount of sp² fraction decreases with density and find 70.0% sp³ with 29.7% sp² and 0.3% sp for 3.4 g/cm³ density, which can be compared to DLC of 3.24 g/cm³ density resulting good agreement with XPS experiments. Based on the simulated 3D structure, we create 2D surface slab consisting of various defective sites within the surface. The 2D surface dominates with hexagonal carbon ring along with few pentagon and heptagon rings in the graphitic structure that may be useful as electrocatalysts for different energy conversion reactions.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1016/j.carbon.2021.07.080DOIArticle
ORCID:
AuthorORCID
Hossain, Md Delowar0000-0003-3440-8306
Cheng, Tao0000-0003-4830-177X
Goddard, William A., III0000-0003-0097-5716
Luo, Zhengtang0000-0002-5134-9240
Additional Information:© 2021 Elsevier Ltd. Received 16 April 2021, Revised 21 July 2021, Accepted 28 July 2021, Available online 3 August 2021. M.D.H and Z.L. acknowledge funds from Research Grant Council of Hong Kong SAR (16304518), NSFC-RGC Joint Research Scheme (N_HKUST607/17), Zhongshan City Bureau of Science and Technology (2019AG018), the IER foundation (HT-JD-CXY-201907). “International science and technology cooperation projects” of Science and Technological Bureau of Guangzhou Huangpu District (2019GH06), Guangdong Science and Technology Department (Project#:2020A0505090003), Research Fund of Guangdong-Hong Kong-Macao Joint Laboratory for Intelligent Micro-Nano Optoelectronic Technology (No. 2020B1212030010). The Caltech efforts were supported by NSF (CBET-1805022) and ONR (N00014-18-1-2155). CRediT authorship contribution statement: Md Delowar Hossain: Conceptualization, Methodology, Investigation, Data analysis, Visualization, Writing – original draft. Qing Zhang: Data analysis, Review & Editing, Discussion. Tao Cheng: Data analysis, Review & Editing, Discussion. William A. Goddard: Supervision, Project administration, and Revision. Zhengtang Luo: Supervision, Project administration, and Revision. All authors approved the final version of the manuscript. The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
Funders:
Funding AgencyGrant Number
Research Grants Council of Hong Kong16304518
National Natural Science Foundation of ChinaN_HKUST607/17
Zhongshan City Bureau of Science and Technology2019AG018
IER FoundationHT-JD-CXY-201907
Science and Technological Bureau of Guangzhou Huangpu District2019GH06
Guangdong Science and Technology Department2020A0505090003
Guangdong-Hong Kong-Macao Joint Laboratory for Intelligent Micro-Nano Optoelectronic Technology2020B1212030010
Subject Keywords:ReaxFF reactive force field; Reactive dynamics simulations; Graphitization; X-ray diffraction; Raman spectroscopy; Carbon electrode
Other Numbering System:
Other Numbering System NameOther Numbering System ID
WAG1483
DOI:10.1016/j.carbon.2021.07.080
Record Number:CaltechAUTHORS:20210823-204347903
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20210823-204347903
Official Citation:Md Delowar Hossain, Qing Zhang, Tao Cheng, William A. Goddard, Zhengtang Luo, Graphitization of low-density amorphous carbon for electrocatalysis electrodes from ReaxFF reactive dynamics, Carbon, Volume 183, 2021, Pages 940-947, ISSN 0008-6223, https://doi.org/10.1016/j.carbon.2021.07.080.
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:110392
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:24 Aug 2021 17:47
Last Modified:19 Oct 2021 18:41

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