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Silicon Radical-Induced CH4 Dissociation for Uniform Graphene Coating on Silica Surface

Pirabul, Kritin; Zhao, Qi; Pan, Zheng-Ze; Liu, Hongyu; Itoh, Mutsuhiro; Izawa, Kenichi; Kawai, Makoto; ... Nishihara, Hirotomo; + view all (2023) Silicon Radical-Induced CH4 Dissociation for Uniform Graphene Coating on Silica Surface. Small , Article e2306325. 10.1002/smll.202306325. (In press). Green open access

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Abstract

Due to the manufacturability of highly well-defined structures and wide-range versatility in its microstructure, SiO2 is an attractive template for synthesizing graphene frameworks with the desired pore structure. However, its intrinsic inertness constrains the graphene formation via methane chemical vapor deposition. This work overcomes this challenge by successfully achieving uniform graphene coating on a trimethylsilyl-modified SiO2 (denote TMS-MPS). Remarkably, the onset temperature for graphene growth dropped to 720 °C for the TMS-MPS, as compared to the 885 °C of the pristine SiO2 . This is found to be mainly from the Si radicals formed from the decomposition of the surface TMS groups. Both experimental and computational results suggest a strong catalytic effect of the Si radicals on the CH4 dissociation. The surface engineering of SiO2 templates facilitates the synthesis of high-quality graphene sheets. As a result, the graphene-coated SiO2 composite exhibits a high electrical conductivity of 0.25 S cm-1 . Moreover, the removal of the TMP-MPS template has released a graphene framework that replicates the parental TMS-MPS template on both micro- and nano- scales. This study provides tremendous insights into graphene growth chemistries as well as establishes a promising methodology for synthesizing graphene-based materials with pre-designed microstructures and porosity.

Type: Article
Title: Silicon Radical-Induced CH4 Dissociation for Uniform Graphene Coating on Silica Surface
Location: Germany
Open access status: An open access version is available from UCL Discovery
DOI: 10.1002/smll.202306325
Publisher version: https://doi.org/10.1002/smll.202306325
Language: English
Additional information: © 2023 The Authors. Small published by Wiley-VCH GmbH This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.
Keywords: CH4 activation, carbon templating, chemical vapor deposition, graphene, silicon radical
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
URI: https://discovery-pp.ucl.ac.uk/id/eprint/10183355
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