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Transfer-free chemical vapor deposition graphene for nitride epitaxy: challenges, current status and future outlook

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Science China Chemistry 2024年第3期67卷 824-840页

作者： Xiang Gao Senlin Li Jingfeng Bi Kaixuan Zhou Meng Li zhongfan liu Jingyu Sun College of Energy Soochow Institute for Energy and Materials InnovationsSUDA-BGI Collaborative Innovation CenterKey Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu ProvinceSoochow UniversitySuzhou 215006China Beijing Graphene Institute Beijing 100095China Xiamen Silan Advanced Compound Semiconductor Co.Ltd. Xiamen 361026China

Graphene, a two-dimensional material with outstanding electrical and mechanical properties, has attracted considerable attention in the field of semiconductor technologies due to its potential use as a buffer layer for the epitaxial Ⅲ-nitride growth. In recent years, significant progress has been made in the chemical vapor deposition growth of graphene on various insulating substrates for the nitride epitaxy, which offers a facile, inexpensive, and easily scalable methodology. However, certain challenges are still present in the form of producing high-quality graphene and achieving optimal interface compatibility with Ⅲ-nitride materials.In this review, we provide an overview of the bottlenecks associated with the transferred graphene fabrication techniques and the state-of-the-art techniques for the transfer-free graphene growth. The present contribution highlights the current progress in the transfer-free graphene growth on different insulating substrates, including sapphire, quartz, SiO_(2)/Si, and discusses the potential applications of transfer-free graphene in the Ⅲ-nitride epitaxy. Finally, it includes the prospects of the transfer-free graphene growth for the Ⅲ-nitride epitaxy and the challenges that should be overcome to realize its full potential in this field.

关键词： Transfer-free chemical vapor deposition graphene for nitride epitaxy challenges current status and future outlook graphene

Theoretical investigations on the growth of graphene by oxygenassisted chemical vapor deposition

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Nano Research 2024年第6期17卷 4645-4650页

作者： Xiaoli Sun Chaojie Yu Yujia Yang Zhihao Li Jianjian Shi Wanjian Yin zhongfan liu Beijing Graphene Institute(BGI) Beijing 100095China School of Physics and Electronics Shandong Normal UniversityJinan 250014China College of Energy Soochow Institute for Energy and Materials InnovationsLight Industry Institute of Electrochemical Power SourcesSUDA-BGI Collaborative Innovation CenterSoochow UniversitySuzhou 215006China School of Electronic Engineering Chengdu Technological UniversityChengdu 611730China Center for Nanochemistry Beijing National Laboratory for Molecular SciencesCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

Recently,graphene has drawn considerable attention in the field of electronics,owing to its favorable conductivity and high carrier mobility.Crucial to the industrialization of graphene is its high-quality microfabrication via chemical vapor deposition.However,many problems remain in its preparation,such as the not fully understood cracking mechanism of the carbon source,the mechanism of its substrate oxidation,and insufficient defect repair theory.To help close this capability gap,this study leverages density functional theory to explore the role of O in graphene growth.The effects of Cu substrate oxidation on carbon source cracking,nucleation barriers,crystal nucleus growth,and defect repairs are discussed.OCu was found to reduce energy change during dehydrogenation,rendering the process easier.Moreover,the adsorbed O in graphene or its Cu substrate can promote defect repair and edge growth.

关键词： density functional theory oxygen-assisted graphene growth chemical vapor deposition Cu substrate

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

Graphene-driving strain engineering to enable strain-free epitaxy of AlN film for deep ultraviolet light-emitting diode

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Light(Science & Applications) 2022年第5期11卷 808-819页

作者： Hongliang Chang Zhetong liu Shenyuan Yang Yaqi Gao Jingyuan Shan Bingyao liu Jingyu Sun Zhaolong Chen Jianchang Yan Zhiqiang liu Junxi Wang Peng Gao Jinmin Li zhongfan liu Tongbo Wei Research and Development Center for Semiconductor Lighting Technology Institute of SemiconductorsChinese Academy of Sciences100083 BeijingChina Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences100049 BeijingChina Center for Nanochemistry(CNC) Beijing Science and Engineering Center for NanocarbonsBeijing National Laboratory for Molecular SciencesCollege of Chemistry and Molecular EngineeringPeking University100871 BeijingChina Electron Microscopy Laboratory and International Center for Quantum MaterialsSchool of PhysicsPeking University100871 BeijingChina Beijing graphene institute(BGI) 100095 BeijingChina Academy for Advanced Interdisciplinary Studies Interdisciplinary Institute of Light-Element Quantum Materials and Research Center for Light-Element Advanced MaterialsPeking University100871 BeijingChina State Key Laboratory of Superlattices and Microstructures Institute of SemiconductorsChinese Academy of Sciences100083 BeijingChina

The energy-efficient deep ultraviolet(DUV)optoelectronic devices suffer from critical issues associated with the poor quality and large strain of nitride material system caused by the inherent mismatch of heteroepitaxy.In this work,we have prepared the strain-free AlN film with low dislocation density(DD)by graphene(Gr)-driving strain-pre-store engineering and a unique mechanism of strain-relaxation in quasi-van der Waals(QvdW)epitaxy is presented.The DD in AlN epilayer with Gr exhibits an anomalous sawtooth-like evolution during the whole epitaxy process.Gr can help to enable the annihilation of the dislocations originated from the interface between AlN and Gr/sapphire by impelling a lateral two-dimensional growth mode.Remarkably,it can induce AlN epilayer to pre-store sufficient tensile strain during the early growth stage and thus compensate the compressive strain caused by hetero-mismatch.Therefore,the low-strain state of the DUV light-emitting diode(DUV-LED)epitaxial structure is realized on the strain-free AlN template with Gr.Furthermore,the DUV-LED with Gr demonstrate 2.1 times enhancement of light output power and a better stability of luminous wavelength compared to that on bare sapphire.An in-depth understanding of this work reveals diverse beneficial impacts of Gr on nitride growth and provides a novel strategy of relaxing the vital requirements of hetero-mismatch in conventional heteroepitaxy.

关键词： sapphire diode strain

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

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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 films.Methane(CH4),has been the most commonly used precursor in the last decade,but it presents challenges in terms of decomposition efficiency and growth rate.Here we thoroughly evaluated acetylene(C2H_(2)),a precursor that is probably for providing carbon dimer(C2)species,for fast growth of large-scale graphene films.We 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 species.Therefore,a C2-fueled scanning growth strategy is proposed,and the fast scanning growth rate of 40 cm/min was experimentally demonstrated.This growth strategy is compatible with the approach of unidirectional growth of single-crystal graphene films,and the as-grown graphene films are of high-quality.This 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

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 films.To 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 mass-transfer.Here,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 min.Computational 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 stacks.This 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

Direct insight into sulfiphilicity-lithiophilicity design of bifunctional heteroatom-doped graphene mediator toward durable Li-S batteries

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Journal of Energy Chemistry 2022年第3期31卷 474-482,I0013页

作者： Haina Ci Menglei Wang Zhongti Sun Chaohui Wei Jingsheng Cai Chen Lu Guang Cui zhongfan liu Jingyu Sun 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 215006JiangsuChina SUDA-BGI Collaborative Innovation Center Soochow UniversitySuzhou 215006JiangsuChina Beijing Graphene Institute(BGI) Beijing 100095China School of Materials Science and Engineering Jiangsu UniversityZhenjiang 212013JiangsuChina Center for Nanochemistry(CNC) Beijing Science and Engineering Center for NanocarbonsCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

The practical applications of lithium-sulfur(Li-S)battery have been greatly hindered by the severe polysulfide shuttle at the cathode and rampant lithium dendrite growth at the anode.One of the effective solutions deals with concurrent management of both electrodes.Nevertheless,this direction remains in a nascent stage due to a lack of material selection and mechanism exploration.Herein,we devise a temperature-mediated direct chemical vapor deposition strategy to realize the controllable synthesis of three-dimensional boron/nitrogen dual-doped graphene(BNG)particulated architectures,which is employed as a light-weighted and multi-functional mediator for both electrodes in Li-S batteries.Benefiting from the“sulfiphilic”and“lithiophilic”features,the BNG modified separator not only enables boosted kinetics of polysulfide transformation to mitigate the shuttle effect but also endows uniform lithium deposition to suppress the dendritic growth.Theoretical calculations in combination with electro-kinetic tests and operando Raman analysis further elucidate the favorable sulfur and lithium electrochemistry of BNG at a molecular level.This work offers direct insight into the mediator design via controllable synthesis of graphene materials to tackle the fundamental challenges of Li-S batteries.

关键词： Li-S batteries B/N dual-doped graphene Mediator Shuttle effect Lithium dendrite

CO_(2)-promoted transfer-free growth of conformal graphene

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Nano Research 2023年第5期16卷 6334-6342页

作者： Ruojuan liu Zhe Peng Xiaoli Sun Zhaolong Chen Zhi Li Haina Ci Bingzhi liu Yi Cheng Bei Jiang Junxiong Hu Wanjian Yin Jingyu Sun zhongfan liu Center for Nanochemistry Beijing National Laboratory for Molecular SciencesCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China Beijing Graphene Institute Beijing 100095China Beijing Cancer Hospital Beijing 100142China Department of Materials Science and Engineering National University of Singapore117575Singapore College of Energy Soochow Institute for Energy and Materials InnovationsSUDA-BGI Collaborative Innovation CenterSoochow UniversitySuzhou 215006China

Gaseous promotors have readily been adopted during the direct synthesis of graphene over insulators to enhance the growth quality and/or boost the growth rate.The understanding of the real functions of carbon-containing promotors has still remained elusive.In this study,we identify the critical roles of a representative CO_(2)promotor played in the direct growth of graphene.The comparative experimental trials validate CO_(2)as an effective modulator to decrease graphene nucleation density,improve growth kinetics,mitigate adlayer formation.The first-principles calculations illustrate that the generation of gas-phase OH species in CO_(2)-assisted system helps decrease the energy barriers of CH4 decomposition and carbon attachment to the growth front,which might be the key factor to allow high-quality direct growth.Such a CO_(2)-promoted strategy enables the conformal coating of graphene film over curved insulators,where the sheet resistance of grown graphene on quartz reaches as low as 1.26 kΩ·sq^(−1)at an optical transmittance of~95.8%.The fabricated endoscope lens based on our conformal graphene harvests an apoptosis of 82.8%for noninvasive thermal therapy.The work presented here is expected to motivate further investigations in the controllable growth of high-quality graphene on insulating substrates.

关键词： chemical vapor deposition graphene carbon dioxide transfer-free growth promotor conformal

Copper acetate-facilitated transfer-free growth of high-quality graphene for hydrovoltaic generators

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National Science Review 2022年第7期9卷 71-79页

作者： Jingyuan Shan Sunmiao Fang Wendong Wang Wen Zhao Rui Zhang Bingzhi liu Li Lin Bei Jiang Haina Ci Ruojuan liu Wen Wang Xiaoqin Yang Wenyue Guo Mark H.Rümmeli Wanlin Guo Jingyu Sun zhongfan liu Center for Nanochemistry (CNC) Beijing Science and Engineering Center for Nanocarbons Beijing National Laboratory for Molecular Sciences College of Chemistry and Molecular Engineering Peking University Academy for Advanced Interdisciplinary Studies Peking University Key Laboratory for Intelligent Nano Materials and Devices of the Ministry of Education State Key Laboratory of Mechanics and Control of Mechanical Structures Institute of Nanoscience Nanjing University of Aeronautics and Astronautics Department of Physics and Astronomy University of Manchester School of Materials Science and Engineering China University of Petroleum (East China) College of Energy Soochow Institute for Energy and Materials Innovations (SIEMIS)Jiangsu Provincial Key Laboratory for Advanced Carbon Materials and Wearable Energy TechnologiesSoochow University Beijing Graphene Institute (BGI)

Direct synthesis of high-quality graphene on dielectric substrates without a transfer process is of vital importance for a variety of applications.Current strategies for boosting high-quality graphene growth,such as remote metal catalyzation,are limited by poor performance with respect to the release of metal catalysts and hence suffer from a problem with metal residues.Herein,we report an effective approach that utilizes a metal-containing species,copper acetate,to continuously supply copper clusters in a gaseous form to aid transfer-free growth of graphene over a wafer scale.The thus-derived graphene films were found to show reduced multilayer density and improved electrical performance and exhibited a carrier mobility of8500 cm~2 V-1s-1.Furthermore,droplet-based hydrovoltaic electricity generator devices based on directly grown graphene were found to exhibit robust voltage output and long cyclic stability,in stark contrast to their counterparts based on transferred graphene,demonstrating the potential for emerging energy harvesting applications.The work presented here offers a promising solution to organize the metal catalytic booster toward transfer-free synthesis of high-quality graphene and enable smart energy generation.

关键词： chemical vapor deposition graphene copper acetate hydrovoltaic electricity generator transfer-free growth