Invisible vapor catalysis in graphene growth by chemical vapor deposition

查看全文 作　　者：Xiucai [1,2]Sun;Xiaoting [1,3]Liu;Zhongti [4]Sun;Xintong [2]Zhang;Yuzhu [1,2]Wu;Yeshu [1,3]Zhu;Yuqing [2]Song;Kaicheng [2]Jia;Jincan [2,5]Zhang;Luzhao [2]Sun;Wan-Jian [2,6]Yin;Zhongfan [1,2]Liu

机构地区：[1]Center for Nanochemistry,Beijing Science and Engineering Center for Nanocarbons,Beijing National Laboratory for Molecular Science,College of Chemistry and Molecular Engineering,Peking University,Beijing 100871,China;[2]Beijing Graphene Institute(BGI),Beijing 100095,China;[3]Academy for Advanced Interdisciplinary Studies,Peking University,Beijing 100871,China;[4]School of Materials Science and Engineering,Jiangsu University,Zhenjiang 212013,China;[5]Department of Engineering,University of Cambridge,Cambridge CB30FA,UK;[6]College of Energy,Soochow Institute for Energy and Materials InnovationS(SIEMIS),Jiangsu Provincial Key Laboratory for Advanced Carbon Materials and Wearable Energy Technologies,Soochow University,Suzhou 215006,China

出　　处：《Nano Research》索引2024年第17卷第5期,共11页

基　　金：supported by the National Natural Science Foundation of China(Nos.T2188101,52021006,52072042);the National Natural Science Foundation of China Youth Scientist Fund(Nos.22105006,52202033);Beijing National Laboratory for Molecular Science(No.BNLMS-CXTD-202001);the National Key R&D Program of China(Nos.2016YFA0200101,2016YFA0200103,2018YFA0703502);the Beijing Municipal Science&Technology Commission(Nos.Z191100000819005,Z191100000819007,Z201100008720005). 摘　　要：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 ambiguous.Here,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 atoms.The 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 catalysis.DFT calculations show Cu clusters,represented by Cu17,have strong capabilities for adsorption,dehydrogenation,and decomposition of hydrocarbons.They 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 graphene.Further experimental validation showed that increasing the amount of Cu vapor improved the as-synthesized graphene growth rate and surface cleanliness.This 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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Invisible vapor catalysis in graphene growth by chemical vapor deposition

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