Graphene Single Crystals: Size and Morphology Engineering
Abstract
Recently developed chemical vapor deposition (CVD) is considered as an effective way to large‐area and high‐quality graphene preparation due to its ultra‐low cost, high controllability, and high scalability. However, CVD‐grown graphene film is polycrystalline, and composed of numerous grains separated by grain boundaries, which are detrimental to graphene‐based electronics. Intensive investigations have been inspired on the controlled growth of graphene single crystals with the absence of intrinsic defects. As the two most concerned parameters, the size and morphology serve critical roles in affecting properties and understanding the growth mechanism of graphene crystals. Therefore, a precise tuning of the size and morphology will be of great significance in scale‐up graphene production and wide applications. Here, recent advances in the synthesis of graphene single crystals on both metals and dielectric substrates by the CVD method are discussed. The review mainly covers the size and morphology engineering of graphene single crystals. Furthermore, recent progress in the growth mechanism and device applications of graphene single crystals are presented. Finally, the opportunities and challenges are discussed.
Citing Literature
Number of times cited according to CrossRef: 67
- Ran Guan, Aiheng Yuan, Birong Luo, Bilayer Graphene: From Stacking Order to Growth Mechanisms, physica status solidi (RRL) – Rapid Research Letters, 10.1002/pssr.201900605, 14, 3, (2020).
- Xia Zhang, Qian Zhou, Miaomiao Yuan, Bin Liao, Xianying Wu, Minju Ying, Etching-controlled preparation of large-area fractal graphene by low-pressure CVD on polycrystalline Cu substrate, Materials Today Communications, 10.1016/j.mtcomm.2020.101093, (101093), (2020).
- Seojoo Lee, Soojeong Baek, Teun‐Teun Kim, Hyukjoon Cho, Sangha Lee, Ji‐Hun Kang, Bumki Min, Metamaterials for Enhanced Optical Responses and their Application to Active Control of Terahertz Waves, Advanced Materials, 10.1002/adma.202000250, 0, 0, (2020).
- Ming Huang, Rodney S. Ruoff, Growth of Single-Layer and Multilayer Graphene on Cu/Ni Alloy Substrates, Accounts of Chemical Research, 10.1021/acs.accounts.9b00643, (2020).
- Svetlana Jovanovic, Graphene Quantum Dots—A New Member of the Graphene Family: Structure, Properties, and Biomedical Applications, Handbook of Graphene Set, 10.1002/9781119468455, (267-299), (2019).
- Chin Wei Lai, Foo Wah Low, Siti Zubaidah Binti Mohamed Siddick, Joon Ching Juan, Graphene/TiO2 Nanocomposites: Synthesis Routes, Characterization, and Solar Cell Applications, Handbook of Graphene Set, 10.1002/9781119468455, (353-394), (2019).
- Jingyuan Zhou, Jiaqiang Li, Zhongfan Liu, Jin Zhang, Exploring Approaches for the Synthesis of Few‐Layered Graphdiyne, Advanced Materials, 10.1002/adma.201803758, 31, 42, (2019).
- Debin Kong, Zhichang Xiao, Yang Gao, Xinghao Zhang, Ruiying Guo, Xiaoxiong Huang, Xianglong Li, Linjie Zhi, Sp2-carbon dominant carbonaceous materials for energy conversion and storage, Materials Science and Engineering: R: Reports, 10.1016/j.mser.2018.10.001, 137, (1-37), (2019).
- Chitengfei Zhang, Rong Tu, Jun Li, Meijun Yang, Qizhong Li, Ji Shi, Haiwen Li, Hitoshi Ohmori, Song Zhang, Lianmeng Zhang, Takashi Goto, Growth of umbrella-like millimeter-scale single-crystalline graphene on liquid copper, Carbon, 10.1016/j.carbon.2019.05.013, (2019).
- Yujing Liu, Ning Liu, Liangmin Yu, Xiaohui Jiang, Xuefeng Yan, Design and Synthesis of Mint Leaf-like Polyacrylonitrile and Carbon Nanosheets for Flexible All-solid-state Asymmetric Supercapacitors, Chemical Engineering Journal, 10.1016/j.cej.2019.01.058, (2019).
- Jianli Li, Ruijue Hu, Hao Qu, Yue Su, Na Wang, Haiquan Su, Xiaojun Gu, Radio-frequency thermal plasma-induced novel chainmail-like core-shell MoO2 as highly stable catalyst for converting syngas to higher alcohols, Applied Catalysis B: Environmental, 10.1016/j.apcatb.2019.02.060, (2019).
- Yingbo Xiao, Jun Huang, Yazhou Xu, Kai Yuan, Yiwang Chen, Facile and Scalable Fabrication of Nitrogen-Doped Porous Carbon Nanosheets for Capacitive Energy Storage with Ultrahigh Energy Density, ACS Applied Materials & Interfaces, 10.1021/acsami.9b04393, (2019).
- Qiqi Zhuo, Yipeng Mao, Suwei Lu, Bolu Cui, Li Yu, Jijun Tang, Jun Sun, Chao Yan, Seed-Assisted Synthesis of Graphene Films on Insulating Substrate, Materials, 10.3390/ma12091376, 12, 9, (1376), (2019).
- Jianing Zhuang, Wen Zhao, Lu Qiu, John Xin, Jichen Dong, Feng Ding, Morphology Evolution of Graphene during Chemical Vapor Deposition Growth: A Phase-Field Theory Simulation, The Journal of Physical Chemistry C, 10.1021/acs.jpcc.9b00761, (2019).
- Xudong Xue, Qiang Xu, Huaping Wang, Shuwei Liu, Qianqing Jiang, Zhiwei Yu, Xiahong Zhou, Tianbao Ma, Liping Wang, Gui Yu, Gas Flow-Driven Aligned Growth of Graphene on Liquid Copper, Chemistry of Materials, 10.1021/acs.chemmater.8b03998, (2019).
- Jie Yang, PingAn Hu, Gui Yu, Design of carbon sources: starting point for chemical vapor deposition of graphene, 2D Materials, 10.1088/2053-1583/ab31bd, 6, 4, (042003), (2019).
- Shuting Zheng, Mengqi Zeng, Hui Cao, Tao Zhang, Xiaowen Gao, Yao Xiao, Lei Fu, Insight into the rapid growth of graphene single crystals on liquid metal via chemical vapor deposition化学气相沉积法在液态金属上快速生长石墨烯单晶, Science China Materials, 10.1007/s40843-019-9406-7, (2019).
- Jinxin Liu, Lei Fu, Controllable Growth of Graphene on Liquid Surfaces, Advanced Materials, 10.1002/adma.201800690, 31, 9, (2018).
- Bing Deng, Zhongfan Liu, Hailin Peng, Toward Mass Production of CVD Graphene Films, Advanced Materials, 10.1002/adma.201800996, 31, 9, (2018).
- Hailong Hu, Maosheng Chen, Yangbin Zhu, Yong Lin, Fushan Li, Tailiang Guo, Structural reconfiguration and stress relaxation in twisted epitaxial graphene by annealing, Nanotechnology, 10.1088/1361-6528/aaef07, 30, 4, (045708), (2018).
- Rebecca F. Albers, Rafael A. Bini, João B. Souza, Derik T. Machado, Laudemir C. Varanda, A general one-pot synthetic strategy to reduced graphene oxide (rGO) and rGO-nanoparticle hybrid materials, Carbon, 10.1016/j.carbon.2018.10.087, (2018).
- Jie Yang, Xihui Qian, Hao Li, Huaping Wang, Xudong Xue, Le Cai, PingAn Hu, Gui Yu, Novel Hollow Graphene Flowers Synthesized by Cu‐Assisted Chemical Vapor Deposition, Advanced Materials Interfaces, 10.1002/admi.201800347, 5, 16, (2018).
- Wenjing Jie, Zhibin Yang, Gongxun Bai, Jianhua Hao, Luminescence in 2D Materials and van der Waals Heterostructures, Advanced Optical Materials, 10.1002/adom.201701296, 6, 10, (2018).
- Afzal Khan, Mohammad Rezwan Habib, Rishi Ranjan Kumar, Sk Masiul Islam, V. Arivazhagan, Muhammad Salman, Deren Yang, Xuegong Yu, Wetting behaviors and applications of metal-catalyzed CVD grown graphene, Journal of Materials Chemistry A, 10.1039/C8TA08325H, (2018).
- Hassan A. Abd El-Rehim, Ahmed R. Tartour, Green synthesis of water dispersied graphene nanosheets using gamma radiation and natural capping agents, Radiation Physics and Chemistry, 10.1016/j.radphyschem.2018.08.027, 153, (208-213), (2018).
- Bang-Bang Jiang, Ming Pan, Chen Wang, Marvin H. Wu, Kizhanipuram Vinodgopal, Gui-Ping Dai, Controllable Synthesis of Circular Graphene Domains by Atmosphere Pressure Chemical Vapor Deposition, The Journal of Physical Chemistry C, 10.1021/acs.jpcc.7b12626, 122, 25, (13572-13578), (2018).
- Bang-Bang Jiang, Ming Pan, Chen Wang, Hua-Fei Li, Ning Xie, Hai-Yan Hu, Fan Wu, Xiao-Ling Yan, Marvin H. Wu, K. Vinodgopal, Gui-Ping Dai, Morphology engineering and etching of graphene domain by low-pressure chemical vapor deposition, Journal of Saudi Chemical Society, 10.1016/j.jscs.2018.06.001, (2018).
- Neha Singh, Suphiya Khan, Nanobioremediation: An Innovative Approach to Fluoride (F) Contamination, Approaches in Bioremediation, 10.1007/978-3-030-02369-0_15, (343-353), (2018).
- Yujing Liu, Xuan Wang, Xiaohui Jiang, Xia Li, Liangmin Yu, Shape-controlled synthesis of porous carbons for flexible asymmetric supercapacitors, Nanoscale, 10.1039/C8NR06966B, (2018).
- Kuo-You Huang, Ang Sheng Chou, Shang-Yi Liu, Wei-Yu Cheng, Chin-Li Hung, Chia-Shuo Li, Mon-Shu Ho, Chih-I Wu, Ultralow-contact-resistance graphene field-effect transistors fabricated with P-type solution doping, Applied Physics Express, 10.7567/APEX.11.075102, 11, 7, (075102), (2018).
- Chao Yu, Xuefeng Guo, Mengqi Shen, Bo Shen, Michelle Muzzio, Zhouyang Yin, Qing Li, Zheng Xi, Junrui Li, Christopher T. Seto, Shouheng Sun, Maximizing the Catalytic Activity of Nanoparticles through Monolayer Assembly on Nitrogen‐Doped Graphene, Angewandte Chemie, 10.1002/ange.201709815, 130, 2, (460-464), (2017).
- Chao Yu, Xuefeng Guo, Mengqi Shen, Bo Shen, Michelle Muzzio, Zhouyang Yin, Qing Li, Zheng Xi, Junrui Li, Christopher T. Seto, Shouheng Sun, Maximizing the Catalytic Activity of Nanoparticles through Monolayer Assembly on Nitrogen‐Doped Graphene, Angewandte Chemie International Edition, 10.1002/anie.201709815, 57, 2, (451-455), (2017).
- Heonjoo Ha, Christopher John Ellison, Polymer/graphene oxide (GO) thermoset composites with GO as a crosslinker, Korean Journal of Chemical Engineering, 10.1007/s11814-017-0250-7, 35, 2, (303-317), (2017).
- Sapanbir S. Thind, Aicheng Chen, Direct Growth of One‐, Two‐, and Three‐Dimensional Nanostructured Materials at Electrode Surfaces, Advances in Electrochemical Science and Engineering, undefined, (97-143), (2017).
- Taegeon Lee, Felisita A Mas’ud, Myung Jong Kim, Heesuk Rho, Spatially resolved Raman spectroscopy of defects, strains, and strain fluctuations in domain structures of monolayer graphene, Scientific Reports, 10.1038/s41598-017-16969-z, 7, 1, (2017).
- Jiewei Chen, Mengqi Cui, Gaoxiang Wu, Tianyue Wang, Joseph Michel Mbengue, Yingfeng Li, Meicheng Li, Fast growth of large single-crystalline graphene assisted by sequential double oxygen passivation, Carbon, 10.1016/j.carbon.2017.01.108, 116, (133-138), (2017).
- Shan Zheng, Guofang Zhong, Xingyi Wu, Lorenzo D'Arsiè, John Robertson, Metal-catalyst-free growth of graphene on insulating substrates by ammonia-assisted microwave plasma-enhanced chemical vapor deposition, RSC Adv., 10.1039/C7RA04162D, 7, 53, (33185-33193), (2017).
- Anna K. Farquhar, Paula A. Brooksby, Robert A.W. Dryfe, Alison J. Downard, Controlled electrodeposition of gold nanoparticles onto copper-supported few-layer graphene in non-aqueous conditions, Electrochimica Acta, 10.1016/j.electacta.2017.03.206, 237, (54-60), (2017).
- Miguel A. Gosálvez, Joseba Alberdi-Rodriguez, Microscopic Origin of the Apparent Activation Energy in Diffusion-Mediated Monolayer Growth of Two-Dimensional Materials, The Journal of Physical Chemistry C, 10.1021/acs.jpcc.7b05794, 121, 37, (20315-20322), (2017).
- Ruiwen Xue, Irfan H. Abidi, Zhengtang Luo, Domain size, layer number and morphology control for graphene grown by chemical vapor deposition, Functional Materials Letters, 10.1142/S1793604717300031, 10, 04, (1730003), (2017).
- Guangwei Geng, Bo Guan, Penglei Chen, Mingshan Zhu, Changchun Yang, Minghua Liu, Highly efficient visible-light-driven plasmonic photocatalysts based on graphene oxide mediated hybridization of graphite and Ag/AgBr, RSC Advances, 10.1039/C6RA27462E, 7, 16, (9948-9957), (2017).
- Hongtao Liu, Yunqi Liu, Controlled Chemical Synthesis in CVD Graphene, Physical Sciences Reviews, 10.1515/psr-2016-0107, 2, 4, (2017).
- Fangzhu Qing, Changqing Shen, Ruitao Jia, Longlong Zhan, Xuesong Li, Catalytic substrates for graphene growth, MRS Bulletin, 10.1557/mrs.2017.237, 42, 11, (819-824), (2017).
- Zhongfan Liu, Li Lin, Huaying Ren, Xiao Sun, CVD Synthesis of Graphene, Thermal Transport in Carbon-Based Nanomaterials, 10.1016/B978-0-32-346240-2.00002-9, (19-56), (2017).
- Sanghamitra Debroy, V. Pavan Kumar, K. Vijaya Sekhar, Swati Ghosh Acharyya, Amit Acharyya, Synergistic effect of temperature and point defect on the mechanical properties of single layer and bi-layer graphene, Superlattices and Microstructures, 10.1016/j.spmi.2017.08.040, (2017).
- Xining Zang, Qin Zhou, Jiyoung Chang, Kwok Siong Teh, Minsong Wei, Alex Zettl, Liwei Lin, Synthesis of Single‐Layer Graphene on Nickel Using a Droplet CVD Process, Advanced Materials Interfaces, 10.1002/admi.201600783, 4, 4, (2017).
- Chitengfei Zhang, Rong Tu, Song Zhang, Jin Huang, Tenghua Gao, Meijun Yang, Qizhong Li, Ji Shi, Lianmeng Zhang, Takashi Goto, Synthesis of large size uniform single-crystalline trilayer graphene on premelting copper, Carbon, 10.1016/j.carbon.2017.06.096, 122, (352-360), (2017).
- S. Sankar, Hwauk Lee, Hyun Jung, Aran Kim, Abu Talha Aqueel Ahmed, Akbar I. Inamdar, Hyungsang Kim, Sejoon Lee, Hyunsik Im, Deuk Young Kim, Ultrathin graphene nanosheets derived from rice husks for sustainable supercapacitor electrodes, New Journal of Chemistry, 10.1039/C7NJ03136J, 41, 22, (13792-13797), (2017).
- Xiao-Ye Wang, Akimitsu Narita, Klaus Müllen, Precision synthesis versus bulk-scale fabrication of graphenes, Nature Reviews Chemistry, 10.1038/s41570-017-0100, 2, 1, (0100), (2017).
- Jung Woo Lee, Sun Woo Kim, Jin Ha Shin, Jong Hwan Park, Seok Hun Kim, Young Il Song, Su Jeong Suh, Observation on the thermal stability of multi-layer graphene with metal nanoparticles with 0D structure, Materials Research Express, 10.1088/2053-1591/aa8f65, 4, 10, (105034), (2017).
- Birong Luo, José M Caridad, Patrick R Whelan, Joachim Dahl Thomsen, David M A Mackenzie, Antonija Grubišić Čabo, Sanjoy K Mahatha, Marco Bianchi, Philip Hofmann, Peter Uhd Jepsen, Peter Bøggild, Timothy J Booth, Sputtering an exterior metal coating on copper enclosure for large-scale growth of single-crystalline graphene, 2D Materials, 10.1088/2053-1583/aa85d5, 4, 4, (045017), (2017).
- Luzhao Sun, Li Lin, Jincan Zhang, Huan Wang, Hailin Peng, Zhongfan Liu, Visualizing fast growth of large single-crystalline graphene by tunable isotopic carbon source, Nano Research, 10.1007/s12274-016-1297-1, 10, 2, (355-363), (2016).
- Li Lin, Luzhao Sun, Jincan Zhang, Jingyu Sun, Ai Leen Koh, Hailin Peng, Zhongfan Liu, Rapid Growth of Large Single‐Crystalline Graphene via Second Passivation and Multistage Carbon Supply, Advanced Materials, 10.1002/adma.201600403, 28, 23, (4671-4677), (2016).
- Kie Yong Cho, Heun Young Seo, Yong Sik Yeom, Pradip Kumar, Albert S. Lee, Kyung-Youl Baek, Ho Gyu Yoon, Stable 2D-structured supports incorporating ionic block copolymer-wrapped carbon nanotubes with graphene oxide toward compact decoration of metal nanoparticles and high-performance nano-catalysis, Carbon, 10.1016/j.carbon.2016.04.049, 105, (340-352), (2016).
- Subash Sharma, Kamal Sharma, Mohamad Saufi Rosmi, Yazid Yaakob, Mona Ibrahim Araby, Hajime Ohtani, Golap Kalita, Masaki Tanemura, Morphology-Controlled Synthesis of Hexagonal Boron Nitride Crystals by Chemical Vapor Deposition, Crystal Growth & Design, 10.1021/acs.cgd.6b01110, 16, 11, (6440-6445), (2016).
- Peter C. Sherrell, Cecilia Mattevi, Mesoscale design of multifunctional 3D graphene networks, Materials Today, 10.1016/j.mattod.2015.12.004, 19, 8, (428-436), (2016).
- Jaehyun Han, Jun-Young Lee, Jong-Souk Yeo, Large-area layer-by-layer controlled and fully bernal stacked synthesis of graphene, Carbon, 10.1016/j.carbon.2016.04.039, 105, (205-213), (2016).
- Chubei Wang, Jianwei Zhou, Feipeng Du, Synthesis of Highly Reduced Graphene Oxide for Supercapacitor, Journal of Nanomaterials, 10.1155/2016/4840301, 2016, (1-7), (2016).
- Hamid Souri, Seong Jun Yu, Hyeonuk Yeo, Munju Goh, Jun-Yeon Hwang, Seung Min Kim, Bon-Cheol Ku, Young Gyu Jeong, Nam-Ho You, A facile method for transparent carbon nanosheets heater based on polyimide, RSC Adv., 10.1039/C6RA07457J, 6, 58, (52509-52517), (2016).
- Susmit Singha Roy, Robert M. Jacobberger, Chenghao Wan, Michael S. Arnold, Controlling the density of pinhole defects in monolayer graphene synthesized via chemical vapor deposition on copper, Carbon, 10.1016/j.carbon.2015.12.089, 100, (1-6), (2016).
- Wei Huang, Zhi-Fei Liu, Zhi-Yong Yang, Top or underneath? Revealing the structure of multilayer graphene domains with atomic force microscopy and theoretical analysis, Carbon, 10.1016/j.carbon.2015.11.072, 99, (131-137), (2016).
- Qi-Long Yan, Michael Gozin, Feng-Qi Zhao, Adva Cohen, Si-Ping Pang, Highly energetic compositions based on functionalized carbon nanomaterials, Nanoscale, 10.1039/C5NR07855E, 8, 9, (4799-4851), (2016).
- M. Vakili, S.M. Hosseinalipour, S. Delfani, S. Khosrojerdi, M. Karami, Experimental investigation of graphene nanoplatelets nanofluid-based volumetric solar collector for domestic hot water systems, Solar Energy, 10.1016/j.solener.2016.02.034, 131, (119-130), (2016).
- Xiangcheng Zhang, Jianan Wang, Weiyao Hu, Kaifu Zhang, Bojing Sun, Guohui Tian, Baojiang Jiang, Kai Pan, Wei Zhou, Facile Strategy to Fabricate Uniform Black TiO2 Nanothorns/Graphene/Black TiO2 Nanothorns Sandwichlike Nanosheets for Excellent Solar‐Driven Photocatalytic Performance, ChemCatChem, 10.1002/cctc.201600934, 8, 20, (3240-3246), (2016).
- Zhixiao Xu, Xiaodong Zhuang, Chongqing Yang, Jing Cao, Zhaoquan Yao, Yanping Tang, Jianzhong Jiang, Dongqing Wu, Xinliang Feng, Nitrogen‐Doped Porous Carbon Superstructures Derived from Hierarchical Assembly of Polyimide Nanosheets, Advanced Materials, 10.1002/adma.201505131, 28, 10, (1981-1987), (2016).
- Huaping Wang, Gui Yu, Direct CVD Graphene Growth on Semiconductors and Dielectrics for Transfer‐Free Device Fabrication, Advanced Materials, 10.1002/adma.201505123, 28, 25, (4956-4975), (2016).
- Jingyu Sun, Yanfeng Zhang, Zhongfan Liu, Direct Chemical Vapor Deposition Growth of Graphene on Insulating Substrates, ChemNanoMat, 10.1002/cnma.201500160, 2, 1, (9-18), (2015).




