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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 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

Near room-temperature ferromagnetism in air-stable twodimensional Cr_(1−x)Te grown by Chemical vapor deposition

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Nano Research 2022年第4期15卷 3763-3769页

作者： Zhansheng Gao Ming Tang Junwei Huang Jiabiao Chen Wei Ai Linglu Wu Xinyue Dong Yifei Ma Zheshan Zhang Lei Zhang Yaping Du Huixia Fu Hongtao Yuan Jinxiong Wu Feng Luo Tianjin Key Lab for Rare Earth Materials and Applications Center for Rare Earth and Inorganic Functional MaterialsSchool of Materials Science and EngineeringNankai UniversityTianjin 300350China National Laboratory of Solid State Microstructures College of Engineering and Applied SciencesNanjing UniversityNanjing 210093China Center of Quantum Materials and Devices&College of Physics Chongqing UniversityChongqing 401331China Beijing National Laboratory for Molecular Sciences Beijing 100871China

Identifying air-stable two-dimensional(2D)ferromagnetism with high Curie temperature(T_(c))is highly desirable for its potential applications in next-generation spintronics.However,most of the work reported so far mainly focuses on promoting one specific key factor of 2D ferromagnetism(T_(c)or air stability),rather than comprehensive promotion of both of them.Herein,ultrathin Cr_(1-x)Te crystals grown by Chemical vapor deposition(CVD)show thickness-dependent T_(c)up to 285 K.The out-of-plane ferromagnetic order is well preserved down to atomically thin limit(2.0 nm),as evidenced by anomalous Hall effect observed in non-encapsulated samples.Besides,the CVD-grown Cr_(1-x)Te nanosheets present excellent ambient stability,with no apparent change in surface roughness or electrical transport properties after exposure to air for months.Our work provides an alternative platform for investigation of intrinsic 2D ferromagnetism and development of innovative spintronic devices.

关键词： Cr1-xTe room-temperature ferromagnetism air stability anomalous Hall effect Chemical vapor deposition

Direct synthesis of moirésuperlattice through Chemical vapor deposition growth of monolayer WS_(2)on plasma-treated HOPG

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Nano Research 2022年第9期15卷 8587-8594页

作者： Xiaowen Zhou Zongnan Zhang Xinlong Zeng Yaping Wu Feiya Xu Chunmiao Zhang Xu Li Zhiming Wu Junyong Kang Department of Physics Engineering Research Center for Micro-Nano Optoelectronic Materials and Devices at Education MinistryOSEDFujian Provincial Key Laboratory of Semiconductor Materials and ApplicationsXiamen UniversityXiamen 361005China

Vertical van der Waals(vdW)heterostructures composed of two-dimensional(2D)layered materials have recently attracted substantial interests due to their unique properties.However,the direct synthesis of moirésuperlattice remains a great challenge due to the difficulties in heterogeneous nucleation on smooth vdW surfaces.Here,we report a controllable Chemical vapor deposition growth of complete monolayer WS_(2)on highly ordered pyrolytic graphite(HOPG)substrates through the plasma pretreatment.The results show that the morphologies of the grown WS_(2)have a strong dependence on the plasma parameters,including gas composition,source power,and treatment time.It is found that the surface C–C bonds are broken in the plasma pretreated HOPG,and the formed small clusters can act as the nucleation sites for the subsequent growth of WS_(2).Moreover,the height of clusters dominates the growth mode of WS_(2)islands.A transition from a 2D mode to three-dimensional(3D)growth mode occurs when the height is higher than the interlayer spacing of the heterostructure.Besides,diverse moirésuperlattices with different twist angles for WS_(2)/HOPG heterostructures are observed,and the formation mechanism is further analyzed by firstprinciples calculations.

关键词： Chemical vapor deposition plasma pretreatment van der Waals(vdW)heterostructures moirésuperlattice

Uniform deposition of ultra-thin TiO_(2) film on mica substrate by atmospheric pressure Chemical vapor deposition: Effect of precursor concentration

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中国化学工程学报:英文版 2023年第8期60卷 99-107页

作者： Ming Liu Ying Li Rui Wang Guoqiang Shao Pengpeng Lv Jun Li Qingshan Zhu State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China School of chemical&Environmental Engineering China University of Mining and Technology-BeijingBeijing 100083China School of chemical Engineering University of Chinese Academy of SciencesBeijing 100049China

The performance of pearlescent pigment significantly affected by the grain size and the roughness of deposited film. The effect of TiCl_(4) concentration on the initial deposition of TiO_(2) on mica by atmospheric pressure Chemical vapor deposition(APCVD) was investigated. The precursor concentration significantly affected the deposition and morphology of TiO_(2) grains assembling the film. The deposition time for fully covering the surface of mica decreased from 120 to 10 s as the TiCl_(4) concentration increased from 0.38%to 2.44%. The grain size increased with the TiCl_(4) concentration. The AFM and TEM analysis demonstrated that the aggregation of TiO_(2) clusters at the initial stage finally result to the agglomeration of fine TiO_(2) grains at high TiCl_(4) concentrations. Following the results, it was suggested that the nucleation density and size was easy to be adjusted when the TiCl_(4) concentration is below 0.90%.

关键词： Chemical vapor deposition TiO_(2)thin film Nucleation reaction Precursor concentration Pearlescent pigment

Chemical vapor deposition synthesis of V-doped MoS2

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Rare Metals 2023年第12期42卷 3985-3992页

作者： Yang Yang Qing-Rong Liang Chun-Li Zhu Guo-Zhong Zheng Jian Zhang Shou-Jun Zheng Yung-Chang Lin De-Zhi Zheng Jia-Dong Zhou School of Physics Beijing Institute of Technology School of Information and Electronics and Advanced Research Institute of Multidisciplinary Science Beijing Institute of Technology School of Physics Shaanxi Normal University The Institute of Scientific and Industrial Research Osaka University Advanced Research Institute of Multidisciplinary Science Beijing Institute of Technology

Van der Waals coupling with different stacking configurations can significantly affect the optical and electronic properties of ultrathin two-dimensional(2D)materials,which is an effective way to tune device performance.Herein,we report a salt-assisted Chemical vapor deposition method for the synthesis of bilayer V-doped MoS2with 2H and 3R phases,which are demonstrated by the second harmonic generation and scanning transmission electron microscopy.Notably,the mobility of the 3R phase V-doped MoS2is 6.2% higher than that of the 2H phase.Through first-principles calculations,we further reveal that this particular behavior is attributed to the stronger interlayer coupling of 3R compared to the 2H stacking configuration.This research can be further generalized to other transition metal chalcogenides and will contribute to the development of electronic devices based on 2D materials in the future.

关键词： Chemical vapor deposition Synthesis First-principles calculations 2H 3R

Direct synthesis of large-area Al-doped graphene by Chemical vapor deposition:Advancing the substitutionally doped graphene family

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Nano Research 2022年第2期15卷 1310-1318页

作者： Sami Ullah Yu Liu Maria Hasan Wenwen Zeng Qitao Shi Xiaoqin Yang Lei Fu Huy Q.Ta Xueyu Lian Jingyu Sun Ruizhi Yang Lijun Liu Mark H.Rummeli College of Energy Soochow Institute for Energy and Materials Innovations Soochow UniversitySuzhou 215006China Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province Soochow UniversitySuzhou 215006China NUTECH School of Applied Sciences&Humanities and Computer Engineering Department National University of TechnologyIslamabad 42000Pakistan Centre of Polymer and Carbon Materials Polish Academy of SciencesM.Curie-Sklodowskiej 34Zabrze 41-819Poland School of Energy and Power Engineering Xian Jiaotong UniversityXian 710049China College of Chemistry and Molecular Science Wuhan UniversityWuhan 430072China Institute for Complex Materials IFW Dresden 20 Helmholtz Strasse Dresden 01069Germany Institute of Environmental Technology VSB-Technical University of Ostrava17.listopadu 15Ostrava 70833Czech Republic

Graphene doping continues to gather momentum because it enables graphene properties to be tuned,thereby affording new properties to,improve the performance of,and expand the application potential of graphene.Graphene can be chemically doped using various methods such as surface functionalization,hybrid composites(e.g.,nanoparticle decoration),and substitution doping,wherein C atoms are replaced by foreign ones in the graphene lattice.Theoretical works have predicted that graphene could be substitutionally doped by aluminum(Al)atoms,which could hold promise for exciting applications,including hydrogen storage and evolution,and supercapacitors.Other theoretical predictions suggest that Al substitutionally doped graphene(AIG)could serve as a material for gas sensors and the catalytic decomposition of undesirable materials.However,fabricating Al substitutionally doped graphene has proven challenging until now.Herein,we demonstrate how controlled-flow Chemical vapor deposition(CVD)implementing a simple solid precursor can yield high-quality and large-area monolayer AIG,and this synthesis is unequivocally confirmed using various characterization methods including local electron energy-loss spectroscopy(EELS).Detailed high-resolution transmission electron microscopy(HRTEM)shows numerous bonding configurations between the Al atoms and the graphene lattice,some of which are not theoretically predicted.Furthermore,the produced AIG shows a CO_(2) capturability superior to those of other substitutionally doped graphenes.

关键词： aluminum-doped graphene single-solid precursor Chemical vapor deposition carbon dioxide capture energy storage catalytic applications

MXene-MoS_(2)nanocomposites via Chemical vapor deposition with enhanced electrocatalytic activity for hydrogen evolution

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Nano Research 2023年第7期16卷 8937-8944页

作者： Ruijie Zhang Yajing Sun Fei Jiao Lin Li Dechao Geng Wenping Hu Tianjin Key Laboratory of Molecular Optoelectronic Sciences Department of ChemistrySchool of ScienceTianjin University and Collaborative Innovation Center of Chemical Science and EngineeringTianjin 300072China College of Chemistry Tianjin Normal UniversityTianjin 300387China

As a new paradigm of material science,two-dimensional(2D)heterostructured composites have attracted extensive interests because of combining the collective advantages and collaborative characteristics of individual building blocks.Molybdenum disulfide(MoS_(2))has demonstrated great promise as a low-cost substitute to platinum-based catalysts for electrochemical hydrogen production.However,the broad adoption of MoS_(2)is hindered by its limited number of active sites and low inherent electrical conductivity.One of the promising methods to further activate MoS_(2)is coupling engineering.Here,we demonstrate for the first time the synthesis of 2D MXene-MoS_(2)nanocomposites through Chemical vapor deposition(CVD)approach,thus leading to precise design in structure type and orientation.The computational results show that nanocomposites have metallic properties.Owing to their unique 2D/2D structure,MXene-MoS_(2)nanocomposites exhibit more active catalytic sites,resulting in higher electrochemical performance,as inherited from parent excellent characteristics,and a much lower overpotential of~69 mV at a current density of 10 mA·cm^(-2) is achieved.This work paves the way to employ CVD method by coupling engineering to construct 2D nanocomposites for energy storage applications.

关键词： MXene molybdenum disulfide(MoS_(2)) Chemical vapor deposition hydrogen evolution reaction

Chemical vapor deposition growth behavior of graphene

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International Journal of Minerals,Metallurgy and Materials 2022年第1期29卷 136-143页

作者： Jie Wang Tengfei Fan Jianchen Lu Xiaoming Cai Lei Gao Jinming Cai Faculty of Materials Science and Engineering Kunming University of Science and TechnologyKunming 650093China Faculty of Mechanical and Electrical Engineering Kunming University of Science and TechnologyKunming 650093China Faculty of Science Kunming University of Science and TechnologyKunming 650093China

The optimized growth parameters of graphene with different morphologies,such as dendrites,rectangle,and hexagon,have been obtained by low-pressure Chemical vapor deposition on polycrystalline copper substrates.The evolution of fractal graphene,which grew on the polycrystalline copper substrate,has also been observed.When the equilibrium growth state of graphene is disrupted,its intrinsic hexagonal symmetry structure will change into a non-hexagonal symmetry structure.Then,we present a systematic and comprehensive study of the evolution of graphene with different morphologies grown on solid copper as a function of the volume ratio of methane to hydrogen in a controllable manner.Moreover,the phenomena of stitching snow-like graphene together and stacking graphene with different angles was also observed.

关键词： graphene Chemical vapor deposition various morphologies dendrites methane

Electronic tattoos based on large-area Mo2C grown by Chemical vapor deposition for electrophysiology

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Nano Research 2023年第3期16卷 4100-4106页

作者： Shiyu Wang Xin Wang Weifeng Zhang Xiaohu Shi Dekui Song Yan Zhang Yan Zhao Zihan Zhao Nan Liu Beijing Graphene Institute Beijing 100094China Beijing Key Laboratory of Energy Conversion and Storage Materials College of ChemistryBeijing Normal UniversityBeijing 100875China

Tattoo electronics has attracted intensive interest in recent years due to its comfortable wearing and imperceivable sensing,and has been broadly applied in wearable healthcare and human-machine interface.However,the tattoo electrodes are mostly composed of metal films and conductive polymers.Two-dimensional(2D)materials,which are superior in conductivity and stability,are barely studied for electronic tattoos.Herein,we reported a novel electronic tattoo based on large-area Mo_(2)C film grown by Chemical vapor deposition(CVD),and applied it to accurately and imperceivably acquire on-body electrophysiological signals and interface with robotics.High-quality Mo_(2)C film was obtained via optimizing the distribution of gas flow during CVD growth.According to the finite element simulation(FES),bottom surface of Cu foil covers more stable gas flow than the top surface,thus leading to more uniform Mo_(2)C film.The resulting Mo_(2)C film was transferred onto tattoo paper,showing a total thickness of~3μm,sheet resistance of 60-150Ω/sq,and skin-electrode impedance of~5×10^(5)Ω.Such thin Mo_(2)C electronic tattoo(MCET in short)can form conformal contact with skin and accurately record electrophysiological signals,including electromyography(EMG),electrocardiogram(ECG),and electrooculogram(EOG).These body signals collected by MCET can not only reflect the health status but also be transformed to control the robotics for human-machine interface.

关键词： electronic tattoo Mo2C film gas flow Chemical vapor deposition electrophysiological signals