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Fast scanning growth of high-quality graphene films on Cu foils fueled by dimeric carbon precursor

Nano Research 2023年第10期16卷 12246-12252页

作者： Heng Chen Xiucai sun Xiaofeng Song Buhang Chen Ziteng Ma Wanjian Yin luzhao sun Zhongfan Liu Center for Nanochemistry Beijing Science and Engineering Center for NanocarbonsBeijing National Laboratory for Molecular SciencesCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China Beijing Graphene Institute Beijing 100095China College of Materials Science and Technology Beijing University of Chemical TechnologyBeijing 100029China College of Energy Soochow Institute for Energy and Materials InnovationS(SIEMIS)Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu ProvinceSUDA-BGI Collaborative Innovation CenterSoochow UniversitySuzhou 215006China

Carbon source precursor is a critical factor governing chemical vapor deposition growth of graphene ***(CH4),has been the most commonly used precursor in the last decade,but it presents challenges in terms of decomposition efficiency and growth *** we thoroughly evaluated acetylene(C2H_(2)),a precursor that is probably for providing carbon dimer(C2)species,for fast growth of large-scale graphene *** find that the graphene growth behaviors fueled by C2H_(2) exhibit unconventional localized growth behavior with significant advantages in terms of high growth rate,which mainly ascribe to the as-decomposed C2 ***,a C2-fueled scanning growth strategy is proposed,and the fast scanning growth rate of 40 cm/min was experimentally *** growth strategy is compatible with the approach of unidirectional growth of single-crystal graphene films,and the as-grown graphene films are of *** work demonstrates a reliable and promising strategy for the rapid synthesis of high-quality graphene film and may pave the avenue to cost-effective mass production of graphene materials in the roll-to-roll system.

关键词： graphene film chemical vapor deposition fast growth carbon dimer roll-to-roll production

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Visualizing fast growth of large single-crystalline graphene by tunable isotopic carbon source

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Nano Research 2017年第2期10卷 355-363页

作者： luzhao sun1 Li Lin Jincan Zhang Huan Wang Hailin Peng Zhongfan Liu Center for Nanochemistry Beijing Science and Engineering Center for Nanocarbons Beijing National Laboratory for Molecular Sciences College of Chemistry and Molecular Engineering Peking University Beijing 100871 China Academy for Advanced Interdisciplinary Studies Peking University Beijing 100871 China

The fast growth of large single-crystalline graphene by chemical vapor deposition on Cu foil remains a challenge for industrial-scale applications. To achieve the fast growth of large single-crystalline graphene, understanding the detailed dynamics governing the entire growth process--including nucleation, growth, and coalescence is important; however, these remain unexplored. In this study, by using a pulsed carbon isotope labeling technique in conjunction with micro-Raman spectroscopy identification, we visualized the growth dynamics, such as nucleation, growth, and coalescence, during the fast growth of large single- crystalline graphene domains. By tuning the supply of the carbon source, a growth rate of 320 μm/min and the growth of centimeter-sized graphene single crystals were achieved on Cu foil.

关键词： large single-crystalline graphene fast growth isotope labelling carbon source

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Theoretical investigations on hydroxyl carbon precursor fueled growth of graphene on transition metal substrates

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Nano Research 2024年第11期17卷 10235-10241页

作者： Chaojie Yu Haiyang Liu Xiaoli sun Jianjian Shi Zhiyu Jing Xiucai sun Yuqing Song Wanjian Yin Guangping Zhang luzhao sun Zhongfan Liu Beijing Graphene Institute Beijing 100095 China School of Physics and Electronics Shandong Normal University Jinan 250014 China Center for Nanochemistry Beijing National Laboratory for Molecular Sciences College of Chemistry and Molecular Engineering Peking University Beijing 100871 China School of Electronic Engineering Chengdu Technological University Chengdu 611730 China Academy for Advanced Interdisciplinary Research School of Instrument and Electronics North University of China Taiyuan 030051 China College of Energy Soochow Institute for Energy and Materials Innovations Soochow University Suzhou 215006 China

Transition metal catalyzed chemical vapor deposition (CVD) is considered as the most promising approach to synthesize highquality graphene films, and low-temperature growth of defect-free graphene films is long-term challenged because of the high energy barrier for precursor dissociation and graphitization. Reducing the growth temperature can also bring advantages on wrinkle-free graphene films owing to the minimized thermal expansion coefficient mismatch. This work focuses on density functional theory (DFT) calculations of the carbon source precursor with hydroxyl group, especially CH_(3)OH, on low-temperature CVD growth of graphene on Cu and CuNi substrate. We calculated all the possible cleavage paths for CH_(3)OH on transition metal substrates. The results show that, firstly, the cleavage barriers of CH_(3)OH on transition metal substrates are slightly lower than those of CH_(4), and once CO appears, it is difficult to break the C-O bond. Secondly, the CO promotes a better formation and retention of perfect rings in the early stage of graphene nucleation and reduces the edge growth barriers. Thirdly, these deoxidation barriers of CO are reduced after CO participates in graphene edge growth. This paper provides a strategy for the lowtemperature growth of wrinkles-free graphene on transition metal substrates using CH_(3)OH.

关键词： density functional theory(DFT) CH3OH Cu(111) CuNi alloys graphene chemical vapor deposition

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Invisible vapor catalysis in graphene growth by chemical vapor deposition

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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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Exploitation of Bi2O2Se/graphene van der Waals heterojunction for creating efficient photodetectors and short-channel field-effect transistors

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InfoMat 2019年第3期1卷 390-395页

作者： Congwei Tan Shipu Xu Zhenjun Tan luzhao sun Jinxiong Wu Tianran Li Hailin Peng Center for Nanochemistry Beijing Science and Engineering Center for NanocarbonsBeijing National Laboratory for Molecular SciencesInstitute of Physical ChemistryCollege of Chemistry and Molecular EngineeringPeking UniversityBeijingChina Academy for Advanced Interdisciplinary Studies Peking UniversityBeijingP.R.China

The formation of heterojunction within solid-state devices enables them with eventually high performances,but provides a challenge for material synthesis and device fabrication because strict conditions such as lattice match are ***,we show a facile method to fabricate a van der Waals(vdW)heterojunction between two-dimensional(2D)bismuth oxyselenide(Bi2O2Se)and graphene,during which the graphene is directly transferred to the Bi2O2Se and served as a lowcontract-resistant electrode with small work function mismatch(~50 meV).As an optoelectronic device,the Bi2O2Se/graphene vdW heterojunction allows for the efficient sensing toward 1200-nm incident *** the application of fieldeffect transistors(FETs),the short-channel(50 nm)sample can be synthesized by utilizing these two 2D materials(ie,channel:Bi2O2Se;drain/source terminal:graphene)and the n-type characteristic can be observed with the accordant field *** is confirmed that we show a simple way to prepare the vdW heterojunction which is aiming to the high-performance applications among optoelectronics and FETs.

关键词： Bi2O2Se graphene van der Waals heterojunctions

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Porous-structure engineered spacer for high-throughput and rapidgrowth of high-quality graphene films

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Nano Research 2022年第11期15卷 9741-9746页

作者： Ziteng Ma Heng Chen Xiaofeng Song Buhang Chen Qin Li Yanglizhi Li Haiyang Liu Kaicheng Jia Shenghong Huang luzhao sun Zhongfan Liu Center for Nanochemistry Beijing Science and Engineering Center for NanocarbonsBeijing National Laboratory for Molecular SciencesCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China Beijing Graphene Institute Beijing 100095China College of Materials Science and Technology Beijing University of Chemical TechnologyBeijing 100029China Academy for Advanced Interdisciplinary Studies Peking UniversityBeijing 100871China College of Energy Soochow Institute for Energy and Materials InnovationS(SIEMIS)Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu ProvinceSoochow UniversitySuzhou 215006China CAS Key Laboratory of Mechanical Behavior and Design of Materials Department of Modern MechanicsUniversity of Science and Technology of ChinaHefei 230027China

Chemical vapor deposition(CVD)in conjunction with batch-to-batch manufacturing process is considered as the most promising technical route for mass-production of high-quality graphene *** improve the space utilization of the CVD chamber and increase the throughput per batch,stacking of the Cu foil substrates is efficient,but suffers from the problems of adjacent fusion and the poor ***,we demonstrate an efficient strategy for high-throughput and rapid growth of high-quality graphene by alternate stacking of Cu foils and porous carbon fiber paper(CFP).Relying on the unhindered mass-transfer through the pores of CFPs,full-covered high-quality graphene films on compact-stacked Cu foils were achieved within 2 *** fluid dynamics(CFD)simulation and isotope labeling technique were performed to explore the gas diffusion and graphene growth process in the confined space of the Cu-CFP *** work provides a feasible method for industrial production of graphene films,which may also be used for batch production of other two-dimensional materials.

关键词： graphene chemical vapor deposition fast growth high-throughput batch-to-batch production

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Toward batch synthesis of high-quality graphene by cold-wall chemical vapor deposition approach

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Nano Research 2022年第11期15卷 9683-9688页

作者： Kaicheng Jia Ziteng Ma Wendong Wang Yongliang Wen Huanxin Li Yeshu Zhu Jiawei Yang Yuqing Song Jiaxin Shao Xiaoting Liu Qi Lu Yixuan Zhao Jianbo Yin luzhao sun Hailin Peng Jincan Zhang Li Lin 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 Beijing 100095China School of Physics and Astronomy University of ManchesterManchester M139PLUK State Key Laboratory for Chemo/Biosensing and Chemometrics College of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082China Department of Engineering University of CambridgeCambridge CB30FAUK Academy for Advanced Interdisciplinary Studies Peking UniversityBeijing 100871China Key Laboratory of Opto-Electronics Technology Ministry of EducationCollege of Electronic Science and TechnologyFaculty of Information TechnologyBeijing University of TechnologyBeijing 100024China State Key Laboratory of Heavy Oil Processing College of ScienceChina University of PetroleumBeijing 102249China School of Materials Science and Engineering Peking UniversityBeijing 100871China

Chemical vapor deposition(CVD)has emerged as a promising approach for the controlled growth of graphene films with appealing scalability,controllability,and ***,the synthesis of high-quality graphene films still suffers from low production capacity and high energy consumption in the conventional hot-wall CVD *** contrast,owing to the different heating mode,cold-wall CVD(CW-CVD)system exhibits promising potential for the industrial-scale production,but the quality of as-received graphene remains inferior with limited domain size and high defect ***,we demonstrated an efficient method for the batch synthesis of high-quality graphene films with millimeter-sized domains based on CW-CVD *** reduced defect density and improved properties,the as-received graphene was proven to be promising candidate material for electronics and anti-corrosion *** study provides a new insight into the quality improvement of graphene derived from CW-CVD system,and paves a new avenue for the industrial production of high-quality graphene films for potential commercial applications.

关键词： graphene cold-wall chemical vapor deposition(CVD) defects electrical performance

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The role of Cu crystallographic orientations towards growing superclean graphene on meter-sized scale

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Nano Research 2022年第4期15卷 3775-3780页

作者： Xiaoting Liu Jincan Zhang Wendong Wang Wei Zhao Heng Chen Bingyao Liu Mengqi Zhang Fushun Liang Lijuan Zhang Rui Zhang Ning Li Yuexin Zhang Yuchen Liu Kaicheng Jia luzhao sun Yixuan Zhao Peng Gao Qinghong Yuan Li Lin Hailin Peng Zhongfan Liu Center for Nanochemistry Beijing Science and Engineering Center for NanocarbonsBeijing National Laboratory for Molecular ScienceCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China Academy for Advanced Interdisciplinary Studies Peking UniversityBeijing 100871China Beijing Graphene Institute Beijing 100095China Department of Engineering University of CambridgeCambridgeCB30FAUK School of Physics and Astronomy University of ManchesterManchesterM139PLUK State Key Laboratory of Precision Spectroscopy School of Physics and Electronic ScienceEast China Normal UniversityShanghai 200241China Electron Microscopy Laboratory and International Center for Quantum Materials School of PhysicsPeking UniversityBeijing 100871China Centre for Theoretical and Computational Molecular Science Australian Institute for Bioengineering and NanotechnologyThe University of QueenslandBrisbaneQLD 4072Australia School of Materials Science and Engineering Peking UniversityBeijing 100871China

Chemical vapor deposition(CVD)-grown graphene films on Cu foils,exhibiting fine scalability and high quality,are still suffering from the adverse impact of surface contamination,i.e.,amorphous *** the recent successful preparation of superclean graphene through Cu-vapor-assisted reactions,the formation mechanism of amorphous carbon remains unclear,especially with regard to the functions of ***,we have found that the crystallographic orientations of underlying metal substrates would determine the cleanness of graphene in such a way that slower diffusion of active carbon species on asformed graphene-Cu(100)surface is the key factor that suppresses the formation of *** facile synthesis of clean graphene is achieved on the meter-sized Cu(100)that is transformed from the polycrystalline Cu ***,a clean surface of graphene on Cu(100)ensures the reduction of transfer-related polymer residues,and enhanced optical and electrical performance,which allows for versatile applications of graphene in biosensors,functioning as flexible transparent *** work would offer a promising material platform for the fundamental investigation and create new opportunities for the advanced applications of high-quality graphene films.

关键词： superclean graphene Cu crystallographic orientations Cu(100)foil improved electrical performance

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Scalable and ultrafast epitaxial growth of single-crystal graphene wafers for electrically tunable liquid-crystal microlens arrays

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Science Bulletin 2019年第10期64卷 659-668页

作者： Bing Deng Zhaowei Xin Ruiwen Xue Shishu Zhang Xiaozhi Xu Jing Gao Jilin Tang Yue Qi Yani Wang Yan Zhao luzhao sun Huihui Wang Kaihui Liu Mark H. Rummeli Lu-Tao Weng Zhengtang Luo Lianming Tong Xinyu Zhang Changsheng Xie Zhongfan Liu Hailin Peng Center for Nanochemistry (CNC) Beijing Science and Engineering Center for Nanocarbons Beijing National Laboratory for Molecular Sciences (BNLMS) College of Chemistry and Molecular Engineering Peking University Beijing 100871 China Beijing Graphene Institute (BCl) Beijing 100094 China Wuhan National Laboratory for Optoelectronics School of Automation National Key Laboratory of Science and Technology on Multispectral Information Processing Huazhong University of Science & Technology Wuhan 430074 China Department of Chemical and Biological Engineering Materials Characterization and Preparation Facility The Hong Kong University of Science and Technology Hong Kong 999077 China State Key Laboratory for Mesoscopic Physics School of Physics Peking University Beijing 100871 China Institute of Functional Nano and Soft Materials (FUNSOM) J iangsu Key Laboratory for Carbon-Based Functional Materials and Devices and Joint International Research Laboratory of Carbon-Based Functional Materials and Devices Soochow University Suzhou 215123 China Academy for Advanced Interdisciplinary Studies Peking University Beijing 100871 China Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province College of Energy Soochow Institute for Energy and Materials Innovations Soochow University Suzhou 215006 China Centre of Polymer and Carbon Materials Polish Academy of Sciences Zabrze 41-819 Poland Wuhan National Laboratory for Optoelectronics Huazhong University of Science & Technology Wuhan 430074 China

The scalable growth of wafer-sized single-crystal graphene in an energy-efficient manner and compatible with wafer process is critical for the killer applications of graphene in high-performance electronics and optoelectronics. Here, ultrafast epitaxial growth of single-crystal graphene wafers is realized on singlecrystal Cu90Ni10(1 1 1) thin films fabricated by a tailored two-step magnetron sputtering and recrystallization process. The minor nickel(Ni) content greatly enhances the catalytic activity of Cu, rendering the growth of a 4 in. single-crystal monolayer graphene wafer in 10 min on Cu90Ni10(1 1 1), 50 folds faster than graphene growth on Cu(1 1 1). Through the carbon isotope labeling experiments, graphene growth on Cu90Ni10(1 1 1) is proved to be exclusively surface-reaction dominated, which is ascribed to the Cu surface enrichment in the Cu Ni alloy, as indicated by element in-depth profile. One of the best benefits of our protocol is the compatibility with wafer process and excellent scalability. A pilot-scale chemical vapor deposition(CVD) system is designed and built for the mass production of single-crystal graphene wafers, with productivity of 25 pieces in one process cycle. Furthermore, we demonstrate the application of single-crystal graphene in electrically controlled liquid-crystal microlens arrays(LCMLA), which exhibit highly tunable focal lengths near 2 mm under small driving voltages. By integration of the graphene based LCMLA and a CMOS sensor, a prototype camera is proposed that is available for simultaneous light-field and light intensity imaging. The single-crystal graphene wafers could hold great promising for highperformance electronics and optoelectronics that are compatible with wafer process.

关键词： Graphene Ultrafast growth CuNi(1 1 1)thin film Single crystal wafer Liquid crystal microlens arrays

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超级蒙烯材料:石墨烯家族的新成员

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物理化学学报 2023年第10期39卷 19-27页

作者：亓月孙禄钊刘忠范北京石墨烯研究院北京100095 北京大学化学与分子工程学院北京100871

超级蒙烯材料是石墨烯材料家族的新成员。通过高温生长过程和巧妙的工艺设计,在传统材料表面沉积连续态石墨烯薄膜。借助高性能石墨烯“蒙皮”,赋予传统材料全新的功能,让原子级厚度的石墨烯薄膜搭乘传统材料载体走进市场。不同于石墨... 详细信息

超级蒙烯材料是石墨烯材料家族的新成员。通过高温生长过程和巧妙的工艺设计,在传统材料表面沉积连续态石墨烯薄膜。借助高性能石墨烯“蒙皮”,赋予传统材料全新的功能,让原子级厚度的石墨烯薄膜搭乘传统材料载体走进市场。不同于石墨烯涂料在材料表面的物理涂敷,这种直接生长的连续态石墨烯“蒙皮”最大程度地保存了石墨烯的本征特性,有着广阔的应用前景。超级蒙烯材料体现了连续态石墨烯薄膜应用的新理念,借助传统材料衬底,解决了超薄石墨烯薄膜的无法自支撑问题,同时回避了金属衬底上薄膜生长的剥离转移难题。由于纳米级到亚微米厚度的石墨烯蒙皮基本上不改变支撑衬底材料的宏观形态,因此超级蒙烯材料具有工艺兼容性强的巨大优势,在不改变现役工程材料加工工艺的前提下发挥其独特的功能,可借力现役工程材料的广阔应用市场,将石墨烯薄膜推向实际应用。超级蒙烯材料可分为蒙烯非金属材料和蒙烯金属材料。按照支撑衬底材料的形态分类,又可细分为蒙烯箔材、蒙烯纤维、蒙烯粉体以及蒙烯泡沫等多种形态,构成琳琅满目的超级蒙烯材料家族。不同形态的超级蒙烯材料进行后加工处理或者与其他材料复合,将进一步丰富超级蒙烯材料家族的内涵。蒙烯玻璃纤维是超级蒙烯材料的典型代表,完美地融合了石墨烯与玻璃纤维的优异性能,已成功用在飞行器的防除冰领域。超级蒙烯材料新概念的提出将有力推动石墨烯与传统材料的融合,为连续态石墨烯薄膜材料的实用化开辟新路,为加快石墨烯材料的产业落地提供新的动力。

关键词：石墨烯化学气相沉积超级蒙烯材料蒙烯金属材料蒙烯非金属材料蒙烯玻璃纤维

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