Controlled growth of Mo<sub>2</sub>C pyramids on liquid Cu surface

Yixuan Fan; Le Huang; Dechao Geng; Wenping Hu

doi:10.1088/1674-4926/41/8/082001

J. Semicond. > 2020, Volume 41 > Issue 8 > 082001

ARTICLES

Controlled growth of Mo₂C pyramids on liquid Cu surface

Yixuan Fan¹, Le Huang², Dechao Geng^1, and Wenping Hu¹

+ Author Affiliations

Corresponding author: Dechao Geng, Email: gengdechao_1987@tju.edu.cn

DOI: 10.1088/1674-4926/41/8/082001

Abstract: Precise spatial control of 2D materials is the key capability of engineering their optical, electronic, and mechanical properties. However, growth of novel 2D Mo₂C on Cu surface by chemical vapor deposition method was revealed to be seed-induced 2D growth, limiting further synthesis of complex Mo₂C spatial structures. In this research, we demonstrate the controlled growth of Mo₂C pyramids with numerous morphologies, which are characterized with clear terraces within the structures. The whole evolution for Mo₂C pyramids in the coursed of CVD process has been detected, posing significant potential in probing growth mechanism. The formation of the Mo₂C pyramids arises from the supersaturation-induced nucleation and concentration-gradient driven diffused growth of a new Mo₂C layer on the edged areas of intrinsic ones, as supported by STEM imaging. This work provides a novel Mo₂C-based pyramid structure and further reveals a sliding growth mechanism, which could offer impetus for the design of new 3D spatial structures of Mo₂C and other 2D materials.

Key words: Mo₂C pyramids, liquid Cu, chemical vapor deposition

References

[1]	Zhang J C, Lin L, Jia K C, et al. Controlled growth of single-crystal graphene films. Adv Mater, 2020, 32, 1903266 doi: 10.1002/adma.201903266
[2]	Liu C, Wang L, Qi J J, et al. Designed growth of large-size 2D single crystals. Adv Mater, 2020, 32, 2000046 doi: 10.1002/adma.202000046
[3]	Cui Y, Li B, Li J B, et al. Chemical vapor deposition growth of two-dimensional heterojunctions. Sci China Phys Mech Astron, 2018, 61, 016801 doi: 10.1007/s11433-017-9105-x
[4]	Kwak W J, Lau K C, Shin C D, et al. A Mo₂C/carbon nanotube composite cathode for lithium-oxygen batteries with high energy efficiency and long cycle life. ACS Nano, 2015, 9, 4129 doi: 10.1021/acsnano.5b00267
[5]	Çakır D, Sevik C, Gülseren O, et al. Mo₂C as a high capacity anode material: A first-principles study. J Mater Chem A, 2016, 4, 6029 doi: 10.1039/C6TA01918H
[6]	Liu Y P, Yu G T, Li G D, et al. Frontispiece: coupling Mo₂C with nitrogen-rich nanocarbon leads to efficient hydrogen-evolution electrocatalytic sites. Angew Chem Int Ed, 2015, 54, 10752 doi: 10.1002/anie.201583761
[7]	Halim J, Kota S, Lukatskaya M R, et al. Synthesis and characterization of 2D molybdenum carbide (MXene). Adv Funct Mater, 2016, 26, 3118 doi: 10.1002/adfm.201505328
[8]	Anasori B, Lukatskaya M R, Gogotsi Y. 2D metal carbides and nitrides (MXenes) for energy storage. Nat Rev Mater, 2017, 2, 16098 doi: 10.1038/natrevmats.2016.98
[9]	Xu C, Wang L B, Liu Z B, et al. Large-area high-quality 2D ultrathin Mo₂C superconducting crystals. Nat Mater, 2015, 14, 1135 doi: 10.1038/nmat4374
[10]	Wang L B, Xu C, Liu Z B, et al. Magnetotransport properties in high-quality ultrathin two-dimensional superconducting Mo₂C crystals. ACS Nano, 2016, 10, 4504 doi: 10.1021/acsnano.6b00270
[11]	Geng D C, Zhao X X, Li L J, et al. Controlled growth of ultrathin Mo₂C superconducting crystals on liquid Cu surface. 2D Mater, 2016, 4, 011012 doi: 10.1088/2053-1583/aa51b7
[12]	Geng D C, Zhao X X, Chen Z X, et al. Direct synthesis of large-area 2D Mo₂C on in situ grown graphene. Adv Mater, 2017, 29, 1700072 doi: 10.1002/adma.201700072
[13]	Deng R X, Zhang H R, Zhang Y H, et al. Graphene/Mo₂C heterostructure directly grown by chemical vapor deposition. Chin Phys B, 2017, 26, 067901 doi: 10.1088/1674-1056/26/6/067901
[14]	Qiao J B, Gong Y, Zuo W J, et al. One-step synthesis of van der Waals heterostructures of graphene and two-dimensional superconducting α-Mo₂C. Phys Rev B, 2017, 95, 201403 doi: 10.1103/PhysRevB.95.201403
[15]	Geng D, Wu B, Guo Y, et al. Uniform hexagonal graphene flakes and films grown on liquid copper surface. PNAS, 2012, 109, 7992 doi: 10.1073/pnas.1200339109
[16]	Wu Y A, Fan Y, Speller S, et al. Large single crystals of graphene on melted copper using chemical vapor deposition. ACS Nano, 2012, 6, 5010 doi: 10.1021/nn3016629
[17]	Zeng M Q, Tan L F, Wang J, et al. Liquid metal: An innovative solution to uniform graphene films. Chem Mater, 2014, 26, 3637 doi: 10.1021/cm501571h
[18]	Wu B, Geng D C, Xu Z P, et al. Self-organized graphene crystal patterns. NPG Asia Mater, 2013, 5, e36 doi: 10.1038/am.2012.68
[19]	Wang Y, Zheng Y, Xu X F, et al. Electrochemical delamination of CVD-grown graphene film: Toward the recyclable use of copper catalyst. ACS Nano, 2011, 5, 9927 doi: 10.1021/nn203700w
[20]	Hÿtch M J, Snoeck E, Kilaas R. Quantitative measurement of displacement and strain fields from HREM micrographs. Ultramicroscopy, 1998, 74, 131 doi: 10.1016/S0304-3991(98)00035-7

Fig. 1. (Color online) Schematic showing the growth of Mo₂C pyramids on liquid Cu substrate.

DownLoad: Full-Size Img PowerPoint

Fig. 2. (Color online) Growth and characterization of Mo₂C pyramids. (a) Crystal and (b, c) electronic structure of Mo₂C from first-principles calculations. (d) Optical images of grown Mo₂C pyramids structures on liquid Cu surface. (e, f) XPS spectra of Mo₂C flake, indicating existence of Mo and C, respectively. (g–i), AFM images of three typical layered pyramids structures.

DownLoad: Full-Size Img PowerPoint

Fig. 3. (Color online) Further characterization and proposed model of Mo₂C pyramid structures. (a) Optical images of grown layered Mo₂C structures on liquid Cu surface and SiO₂/Si substrate. (b) Raman spectrum of Mo₂C flake, having characterized peak at around 650 cm^–1. (c, d) Optical image of broken layered Mo₂C structure, with bare hexagonal profile of Cu left.

DownLoad: Full-Size Img PowerPoint

Fig. 4. (Color online) Growth of novel Mo₂C pyramid structures. (a) Optical images of the large-area as-grown Mo₂C structures on liquid Cu surface and transferred onto SiO₂/Si substrate, respectively. (b) AFM image of the single structure, displaying clear layered feature. The inset shows height profile of the structure, showing step feature across the whole flake reflected in thickness. (c–f) Optical images of the growth process of Mo₂C structures, showing the time-dependent feature. (g) Schematic diagram illustrates the growth of novel layered Mo₂C structures, corresponding to the observations in (c–f).

DownLoad: Full-Size Img PowerPoint

Fig. 5. (Color online) STEM characterization of Mo₂C pyramid. (a) STEM-ADF image of a typical edge region in the Mo₂C pyramids structures. (b) Strain field mapping based on the image shown in (a).

DownLoad: Full-Size Img PowerPoint

[1]	Zhang J C, Lin L, Jia K C, et al. Controlled growth of single-crystal graphene films. Adv Mater, 2020, 32, 1903266 doi: 10.1002/adma.201903266
[2]	Liu C, Wang L, Qi J J, et al. Designed growth of large-size 2D single crystals. Adv Mater, 2020, 32, 2000046 doi: 10.1002/adma.202000046
[3]	Cui Y, Li B, Li J B, et al. Chemical vapor deposition growth of two-dimensional heterojunctions. Sci China Phys Mech Astron, 2018, 61, 016801 doi: 10.1007/s11433-017-9105-x
[4]	Kwak W J, Lau K C, Shin C D, et al. A Mo₂C/carbon nanotube composite cathode for lithium-oxygen batteries with high energy efficiency and long cycle life. ACS Nano, 2015, 9, 4129 doi: 10.1021/acsnano.5b00267
[5]	Çakır D, Sevik C, Gülseren O, et al. Mo₂C as a high capacity anode material: A first-principles study. J Mater Chem A, 2016, 4, 6029 doi: 10.1039/C6TA01918H
[6]	Liu Y P, Yu G T, Li G D, et al. Frontispiece: coupling Mo₂C with nitrogen-rich nanocarbon leads to efficient hydrogen-evolution electrocatalytic sites. Angew Chem Int Ed, 2015, 54, 10752 doi: 10.1002/anie.201583761
[7]	Halim J, Kota S, Lukatskaya M R, et al. Synthesis and characterization of 2D molybdenum carbide (MXene). Adv Funct Mater, 2016, 26, 3118 doi: 10.1002/adfm.201505328
[8]	Anasori B, Lukatskaya M R, Gogotsi Y. 2D metal carbides and nitrides (MXenes) for energy storage. Nat Rev Mater, 2017, 2, 16098 doi: 10.1038/natrevmats.2016.98
[9]	Xu C, Wang L B, Liu Z B, et al. Large-area high-quality 2D ultrathin Mo₂C superconducting crystals. Nat Mater, 2015, 14, 1135 doi: 10.1038/nmat4374
[10]	Wang L B, Xu C, Liu Z B, et al. Magnetotransport properties in high-quality ultrathin two-dimensional superconducting Mo₂C crystals. ACS Nano, 2016, 10, 4504 doi: 10.1021/acsnano.6b00270
[11]	Geng D C, Zhao X X, Li L J, et al. Controlled growth of ultrathin Mo₂C superconducting crystals on liquid Cu surface. 2D Mater, 2016, 4, 011012 doi: 10.1088/2053-1583/aa51b7
[12]	Geng D C, Zhao X X, Chen Z X, et al. Direct synthesis of large-area 2D Mo₂C on in situ grown graphene. Adv Mater, 2017, 29, 1700072 doi: 10.1002/adma.201700072
[13]	Deng R X, Zhang H R, Zhang Y H, et al. Graphene/Mo₂C heterostructure directly grown by chemical vapor deposition. Chin Phys B, 2017, 26, 067901 doi: 10.1088/1674-1056/26/6/067901
[14]	Qiao J B, Gong Y, Zuo W J, et al. One-step synthesis of van der Waals heterostructures of graphene and two-dimensional superconducting α-Mo₂C. Phys Rev B, 2017, 95, 201403 doi: 10.1103/PhysRevB.95.201403
[15]	Geng D, Wu B, Guo Y, et al. Uniform hexagonal graphene flakes and films grown on liquid copper surface. PNAS, 2012, 109, 7992 doi: 10.1073/pnas.1200339109
[16]	Wu Y A, Fan Y, Speller S, et al. Large single crystals of graphene on melted copper using chemical vapor deposition. ACS Nano, 2012, 6, 5010 doi: 10.1021/nn3016629
[17]	Zeng M Q, Tan L F, Wang J, et al. Liquid metal: An innovative solution to uniform graphene films. Chem Mater, 2014, 26, 3637 doi: 10.1021/cm501571h
[18]	Wu B, Geng D C, Xu Z P, et al. Self-organized graphene crystal patterns. NPG Asia Mater, 2013, 5, e36 doi: 10.1038/am.2012.68
[19]	Wang Y, Zheng Y, Xu X F, et al. Electrochemical delamination of CVD-grown graphene film: Toward the recyclable use of copper catalyst. ACS Nano, 2011, 5, 9927 doi: 10.1021/nn203700w
[20]	Hÿtch M J, Snoeck E, Kilaas R. Quantitative measurement of displacement and strain fields from HREM micrographs. Ultramicroscopy, 1998, 74, 131 doi: 10.1016/S0304-3991(98)00035-7

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Received: 20 May 2020 Revised: 26 May 2020 Online: Accepted Manuscript: 22 June 2020Uncorrected proof: 28 June 2020Published: 04 August 2020

Article Navigation > Journal of Semiconductors > 2020 > 41(8): 082001

Yixuan Fan, Le Huang, Dechao Geng, Wenping Hu. Controlled growth of Mo2C pyramids on liquid Cu surface[J]. Journal of Semiconductors, 2020, 41(8): 082001. doi: 10.1088/1674-4926/41/8/082001 ****Y X Fan, L Huang, D C Geng, W P Hu, Controlled growth of Mo2C pyramids on liquid Cu surface[J]. J. Semicond., 2020, 41(8): 082001. doi: 10.1088/1674-4926/41/8/082001.

Citation:

Yixuan Fan, Le Huang, Dechao Geng, Wenping Hu. Controlled growth of Mo₂C pyramids on liquid Cu surface[J]. Journal of Semiconductors, 2020, 41(8): 082001. doi: 10.1088/1674-4926/41/8/082001 ****

Y X Fan, L Huang, D C Geng, W P Hu, Controlled growth of Mo2C pyramids on liquid Cu surface[J]. J. Semicond., 2020, 41(8): 082001. doi: 10.1088/1674-4926/41/8/082001.

Citation:

Yixuan Fan, Le Huang, Dechao Geng, Wenping Hu. Controlled growth of Mo₂C pyramids on liquid Cu surface[J]. Journal of Semiconductors, 2020, 41(8): 082001. doi: 10.1088/1674-4926/41/8/082001 ****

Y X Fan, L Huang, D C Geng, W P Hu, Controlled growth of Mo2C pyramids on liquid Cu surface[J]. J. Semicond., 2020, 41(8): 082001. doi: 10.1088/1674-4926/41/8/082001.

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Controlled growth of Mo₂C pyramids on liquid Cu surface

DOI: 10.1088/1674-4926/41/8/082001

1.
Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, School of Science, Tianjin University and Collaborative Innovation Center of Chemical Science and Engineering, Tianjin 300072, China
2.
School of Materials and Energy, Guangdong University of Technology, Guangzhou 510006, China

More Information

Corresponding author: Email: gengdechao_1987@tju.edu.cn
Received Date: 2020-05-20
Revised Date: 2020-05-26
Published Date: 2020-08-09

Abstract

Abstract

Precise spatial control of 2D materials is the key capability of engineering their optical, electronic, and mechanical properties. However, growth of novel 2D Mo₂C on Cu surface by chemical vapor deposition method was revealed to be seed-induced 2D growth, limiting further synthesis of complex Mo₂C spatial structures. In this research, we demonstrate the controlled growth of Mo₂C pyramids with numerous morphologies, which are characterized with clear terraces within the structures. The whole evolution for Mo₂C pyramids in the coursed of CVD process has been detected, posing significant potential in probing growth mechanism. The formation of the Mo₂C pyramids arises from the supersaturation-induced nucleation and concentration-gradient driven diffused growth of a new Mo₂C layer on the edged areas of intrinsic ones, as supported by STEM imaging. This work provides a novel Mo₂C-based pyramid structure and further reveals a sliding growth mechanism, which could offer impetus for the design of new 3D spatial structures of Mo₂C and other 2D materials.
- Mo₂C pyramids,
- liquid Cu,
- chemical vapor deposition

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References(20)

References

[1]	Zhang J C, Lin L, Jia K C, et al. Controlled growth of single-crystal graphene films. Adv Mater, 2020, 32, 1903266 doi: 10.1002/adma.201903266
[2]	Liu C, Wang L, Qi J J, et al. Designed growth of large-size 2D single crystals. Adv Mater, 2020, 32, 2000046 doi: 10.1002/adma.202000046
[3]	Cui Y, Li B, Li J B, et al. Chemical vapor deposition growth of two-dimensional heterojunctions. Sci China Phys Mech Astron, 2018, 61, 016801 doi: 10.1007/s11433-017-9105-x
[4]	Kwak W J, Lau K C, Shin C D, et al. A Mo₂C/carbon nanotube composite cathode for lithium-oxygen batteries with high energy efficiency and long cycle life. ACS Nano, 2015, 9, 4129 doi: 10.1021/acsnano.5b00267
[5]	Çakır D, Sevik C, Gülseren O, et al. Mo₂C as a high capacity anode material: A first-principles study. J Mater Chem A, 2016, 4, 6029 doi: 10.1039/C6TA01918H
[6]	Liu Y P, Yu G T, Li G D, et al. Frontispiece: coupling Mo₂C with nitrogen-rich nanocarbon leads to efficient hydrogen-evolution electrocatalytic sites. Angew Chem Int Ed, 2015, 54, 10752 doi: 10.1002/anie.201583761
[7]	Halim J, Kota S, Lukatskaya M R, et al. Synthesis and characterization of 2D molybdenum carbide (MXene). Adv Funct Mater, 2016, 26, 3118 doi: 10.1002/adfm.201505328
[8]	Anasori B, Lukatskaya M R, Gogotsi Y. 2D metal carbides and nitrides (MXenes) for energy storage. Nat Rev Mater, 2017, 2, 16098 doi: 10.1038/natrevmats.2016.98
[9]	Xu C, Wang L B, Liu Z B, et al. Large-area high-quality 2D ultrathin Mo₂C superconducting crystals. Nat Mater, 2015, 14, 1135 doi: 10.1038/nmat4374
[10]	Wang L B, Xu C, Liu Z B, et al. Magnetotransport properties in high-quality ultrathin two-dimensional superconducting Mo₂C crystals. ACS Nano, 2016, 10, 4504 doi: 10.1021/acsnano.6b00270
[11]	Geng D C, Zhao X X, Li L J, et al. Controlled growth of ultrathin Mo₂C superconducting crystals on liquid Cu surface. 2D Mater, 2016, 4, 011012 doi: 10.1088/2053-1583/aa51b7
[12]	Geng D C, Zhao X X, Chen Z X, et al. Direct synthesis of large-area 2D Mo₂C on in situ grown graphene. Adv Mater, 2017, 29, 1700072 doi: 10.1002/adma.201700072
[13]	Deng R X, Zhang H R, Zhang Y H, et al. Graphene/Mo₂C heterostructure directly grown by chemical vapor deposition. Chin Phys B, 2017, 26, 067901 doi: 10.1088/1674-1056/26/6/067901
[14]	Qiao J B, Gong Y, Zuo W J, et al. One-step synthesis of van der Waals heterostructures of graphene and two-dimensional superconducting α-Mo₂C. Phys Rev B, 2017, 95, 201403 doi: 10.1103/PhysRevB.95.201403
[15]	Geng D, Wu B, Guo Y, et al. Uniform hexagonal graphene flakes and films grown on liquid copper surface. PNAS, 2012, 109, 7992 doi: 10.1073/pnas.1200339109
[16]	Wu Y A, Fan Y, Speller S, et al. Large single crystals of graphene on melted copper using chemical vapor deposition. ACS Nano, 2012, 6, 5010 doi: 10.1021/nn3016629
[17]	Zeng M Q, Tan L F, Wang J, et al. Liquid metal: An innovative solution to uniform graphene films. Chem Mater, 2014, 26, 3637 doi: 10.1021/cm501571h
[18]	Wu B, Geng D C, Xu Z P, et al. Self-organized graphene crystal patterns. NPG Asia Mater, 2013, 5, e36 doi: 10.1038/am.2012.68
[19]	Wang Y, Zheng Y, Xu X F, et al. Electrochemical delamination of CVD-grown graphene film: Toward the recyclable use of copper catalyst. ACS Nano, 2011, 5, 9927 doi: 10.1021/nn203700w
[20]	Hÿtch M J, Snoeck E, Kilaas R. Quantitative measurement of displacement and strain fields from HREM micrographs. Ultramicroscopy, 1998, 74, 131 doi: 10.1016/S0304-3991(98)00035-7

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Controlled growth of Mo₂C pyramids on liquid Cu surface

Controlled growth of Mo₂C pyramids on liquid Cu surface