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Invisible vapor catalysis in graphene growth by chemical vapor deposition

Nano Research 2024年第5期17卷 4259-4269页

作者： Xiucai Sun Xiaoting Liu Zhongti Sun Xintong Zhang Yuzhu Wu Yeshu Zhu Yuqing Song Kaicheng Jia Jincan Zhang Luzhao Sun Wan-Jian Yin Zhongfan Liu Center for Nanochemistry Beijing Science and Engineering Center for NanocarbonsBeijing National Laboratory for Molecular ScienceCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China Beijing Graphene Institute(BGI) Beijing 100095China Academy for Advanced Interdisciplinary Studies Peking UniversityBeijing 100871China School of Materials Science and Engineering Jiangsu UniversityZhenjiang 212013China Department of Engineering University of CambridgeCambridge CB30FAUK College of Energy Soochow Institute for Energy and Materials InnovationS(SIEMIS)Jiangsu Provincial Key Laboratory for Advanced Carbon Materials and Wearable Energy TechnologiesSoochow UniversitySuzhou 215006China

vapor catalysis was recently found to play a crucial role in superclean graphene growth via chemical vapor decomposition(CVD).However,knowledge of vapor-phase catalysis is scarce,and several fundamental issues,including vapor compositions and their impact on graphene growth,are ***,by combining density functional theory(DFT)calculations,an ideal gas model,and a designed experiment,we found that the vapor was mainly composed of Cui clusters with tens of *** vapor pressure was estimated to be~10^(-12)-10^(-1)1 bar under normal low-pressure CVD system(LPCVD)conditions for graphene growth,and the exposed surface area of Cui clusters in the vapor was 22-269 times that of the Cu substrate surface,highlighting the importance of vapor *** calculations show Cu clusters,represented by Cu17,have strong capabilities for adsorption,dehydrogenation,and decomposition of *** exhibit an adsorption lifetime and reaction flux six orders of magnitude higher than those on the Cu surface,thus providing a sufficient supply of active C atoms for rapid graphene growth and improving the surface cleanliness of the synthesized *** experimental validation showed that increasing the amount of Cu vapor improved the as-synthesized graphene growth rate and surface *** study provides a comprehensive understanding of vapor catalysis and the fundamental basis of vapor control for superclean graphene rapid growth.

关键词： vapor catalysis graphene growth chemical vapor deposition first-principles calculation

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