共形二维材料: 创制与应用

doi:10.6023/A24070219

化学学报 ›› 2024, Vol. 82 ›› Issue (11): 1162-1179.DOI: 10.6023/A24070219 上一篇下一篇

综述

共形二维材料: 创制与应用

刘卫涛^a, 高战胜^a, 黄明举^a, 刘忠范^b^,^c^,^*(), 陈珂^a^,^d^,^*()

a 河南大学低维材料物理研究中心物理与电子学院未来技术学院开封 475004
b 北京大学化学与分子工程学院北京 100871
c 北京石墨烯研究院北京 100095
d 河南省科学院量子材料与物理研究所郑州 450046

投稿日期:2024-07-17 发布日期:2024-10-08

作者简介:

刘卫涛, 河南大学物理与电子学院在读博士生. 2018年毕业于郑州航空工业管理学院应用物理学专业, 同年进入河南大学物理与电子学院攻读硕士学位并于2020年转入硕博连读, 师从陈珂教授和黄明举教授. 研究方向为二维材料的生长调控与应用.

高战胜, 博士, 2023年毕业于南开大学材料学院, 同年入职河南大学物理与电子学院, 主要研究方向为低维材料及其异质结合成与器件表征.

黄明举, 博士, 河南大学教授. 河南省物理学会理事, 中国光学学会光学材料专业委员会委员, 国家高等学校“光电信息工程”类专业教学指导委员会协作分会委员, Opt. Eng.、Chin. Phys. Lett.、中国激光、光子学报等专业期刊审稿人. 河南省教育厅学术带头人, 省高校优秀骨干教师. 先后主持和参加国家自然科学基金等省部级以上项目11项, 获省部级以上优秀奖4项. 共发表SCI、EI论文160余篇.

刘忠范, 物理化学家, 日本东京大学博士. 北京大学博士生导师、博雅讲席教授、纳米科学与技术研究中心主任, 北京石墨烯研究院院长. 中国科学院院士、发展中国家科学院院士. 英国物理学会会士、英国皇家化学会会士、中国微米纳米技术学会会士. “物理化学学报”主编、“科学通报”副主编. 主要从事石墨烯等纳米碳材料研究, 在石墨烯、碳纳米管的化学气相沉积生长方法研究领域做出了一系列开拓性和引领性的工作. 发表SCI检索学术论文550余篇, 申请中国发明专利80余项. 曾获日中科技交流协会“有山兼孝纪念研究奖”(1992)、香港求是科技基金会杰出青年学者奖(1997)、中国分析测试协会科学技术奖一等奖(2005)、教育部高等学校科学技术奖自然科学一等奖(2007)、国家自然科学二等奖(2008)、中国化学会-阿克苏诺贝尔化学奖(2012)、宝钢优秀教师特等奖(2012)、日本化学会胶体与界面化学年会Lectureship Award(2016)、北京大学方正教师特别奖(2016)、“北京市优秀教师”称号(2017)、国家自然科学二等奖(2017)、ACS Nano Lectureship Award(2018)等.

陈珂, 河南大学教授, 博导, 国家万人计划青年拔尖人才(2020). 2012年获同济大学材料物理与化学博士学位并于同年入职河南大学. 2012年在英国剑桥大学化学系做访问博士生. 2013~2018年在北京大学化学与分子工程学院做博士后和访问学者. 2020~2021年在美国麻省理工学院材料科学与工程系做访问学者. 研究方向为二维材料的可控生长与纳米光学. 在Nat. Photon.、Nat. Commun.、Adv. Mater.等国际著名期刊共发表SCI论文60余篇, 参与编写石墨烯相关专著(章节)2部, 授权国家发明专利8项. 获河南省中原基础研究领军人才、中原青年拔尖人才、省教育厅学术技术带头人、省优秀青年专家、河南省青年科技奖等称号或奖励.

基金资助:
国家自然科学基金(52272038); 国家自然科学基金(22309042); 国家万人计划和河南省中原英才计划的资助

Conformal Two-Dimensional Materials: Preparation and Applications

Weitao Liu^a, Zhansheng Gao^a, Mingju Huang^a, Zhongfan Liu^b^,^c(), Ke Chen^a^,^d()

a Center for the Physics of Low-Dimensional Materials, School of Physics and Electronics, School of Future Technology, Henan University, Kaifeng 475004, China
b College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China
c Beijing Graphene Institute, Beijing 100095, China
d Institute of Quantum Materials and Physics, Henan Academy of Sciences, Zhengzhou 450046, China

Received:2024-07-17 Published:2024-10-08
Contact: ^*E-mail: kchen@henu.edu.cn; zfliu@pku.edu.cn
Supported by:
National Natural Science Foundation of China(52272038); National Natural Science Foundation of China(22309042); National Young Top-Notch Talents of Ten-Thousand Talents Program and the Zhongyuan Talents Program of Henan Province

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摘要/Abstract

共形二维材料是指能与任意基底的表面形状“紧密贴合”的原子薄层材料, 它像薄膜一样紧密包覆于基底表面, 与基底表面轮廓融为一体, 进而形成一种新型的功能复合结构材料. 这种共形结构材料不仅继承了基底原始的表面形貌特征, 而且能将二维材料的新奇物性赋予基底材料而实现新的功能, 激发二维材料与基底相互作用下新的物理化学效应. 基底特殊结构的引入能够使二维材料超越二维空间的局限性, 将二维材料的平面结构与基底的任意曲面结构相结合, 是增强二维材料与外界物质相互作用的重要方式, 极大地拓展了二维材料的应用场景, 甚至可能实现其“杀手锏”应用. 本综述在提出共形二维材料概念的基础上, 阐明了二维材料共形生长的机制, 揭示了基底属性、结构对二维材料共形生长与共形度的影响规律, 探究了影响材料生长行为的热动力学因素与空间相平衡条件, 并分类综述了以基底的开放式结构和限域式结构为典型代表的共形二维材料的制备方法、性能与应用, 最后对该领域的挑战和未来发展方向做了展望.

关键词: 二维材料, 共形生长, 共形度, 开放结构, 限域结构

Conformal two-dimensional materials refer to an atomically-thin layered material that can closely adhere on the surface of any substrate. It is tightly coated on the substrate surface like a thin film, along with the contour of the substrate surface, and thus forms a new type of functional composite structural material. This conformal structural material not only inherits the original surface morphological characteristics of the substrate, but also endows the substrate with novel physical properties of two-dimensional materials to achieve new functions and stimulate new physical and chemical effects under the interaction between two-dimensional materials and the substrate. The introduction of special substrate structures can enable two-dimensional materials to transcend the limitations of two-dimensional space. Combining the planar structure of two-dimensional materials with the arbitrary curved structure of the substrate is an important way to enhance interactions between two-dimensional materials and the surrounding environment, greatly expanding the application fields of two-dimensional materials, and may even achieve the killer applications. On the basis of proposing the concept of conformal two-dimensional materials, this article first elucidates the mechanism of conformal growth of two-dimensional materials, reveals the influence of substrate features and structures on the conformal growth and conformity of two-dimensional materials, as well as explores the thermodynamic factors and spatial equilibrium conditions that affect material growth behaviors. Second, it classifies and summarizes current progress on the preparation methods, properties, and applications of conformal two-dimensional materials represented by open and confined structures of substrates. Finally, the challenges and future development directions in this field are discussed.

Key words: two-dimensional material, conformal growth, conformality, open architecture, confined architecture

引用此文

刘卫涛, 高战胜, 黄明举, 刘忠范, 陈珂. 共形二维材料: 创制与应用[J]. 化学学报, 2024, 82(11): 1162-1179.

Weitao Liu, Zhansheng Gao, Mingju Huang, Zhongfan Liu, Ke Chen. Conformal Two-Dimensional Materials: Preparation and Applications[J]. Acta Chimica Sinica, 2024, 82(11): 1162-1179.

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图/表 16

图1. 共形二维材料与共形包覆示意图

Figure 1. Schematic of conformal 2D materials and conformal coating

图2. 共形度示意图

Figure 2. Schematic of conformity

图3. 金属基底上石墨烯的生长过程

Figure 3. Schematic of growth processes of graphene on metal substrates

图4. 平面和凹角基底上的成核过程. (a)光滑平面基底上的非均匀成核. (b)成核功形状因子f(θ)与浸润角的函数关系. (c)凹陷界面上的非均匀成核. (d)不同凹陷角φ下成核功形状因子f与浸润角度θ的函数关系

Figure 4. Nucleation process on flat and concave substrates. (a) Non-uniform nucleation on a smooth planar substrate. (b) Nucleation work shape factor f(θ) as a function of infiltration angle. (c) Non-uniform nucleation on the concave interface. (d) The functional relationship between the nucleation work shape factor f and the infiltration angle θ under different concave angles φ

图5. 球冠状弯曲界面及其引起的附加压力

Figure 5. Curved interface of spherical corona and the additional pressure

图6. 粗糙基底上晶核生长过程. (a)原子沉积、蒸发、扩散、吸附、脱附、成核、长大的过程. (b)简单立方晶系(100)面上原子可沉积位置示意图. (c)粗糙界面连续生长过程原子跃迁的势能

Figure 6. The growth process of crystal nuclei on rough substrates. (a) Processes of atom deposition, evaporation, diffusion, adsorption, desorption, as well as nucleation and growth. (b) Schematic of the deposition positions of atoms on (100) plane of a simple cubic crystal. (c) Potential energy of atom transition on the rough interface during the continuous crystal growth process

图7. 不同曲面结构上二维材料的生长行为

Figure 7. Growth behavior of 2D materials on different curved surface structures

图8. 限域空间对流体的影响. (a)边界层内的流速分布. (b)不同雷诺数绕圆柱体的流动. (c)管状孔内气体的流动. (d)不同压强下4 μm孔径PCF内生长石墨烯时气体的流动形式

Figure 8. Influence of the confined space on fluid behaviors. (a) Distribution of flow velocity within the boundary layer. (b) Schematic of gas flow around a cylinder at different Reynolds numbers. (c) Schematic of gas flows within a tube. (d) Schematic of gas flows during the graphene growth process in PCF with pore diameter of ca. 4 μm at different pressures

图9. 二维材料的开放式共形结构. (a)被二维MoS2覆盖的SiO2微球示意图[95]. (b) Au/SiO2纳米颗粒的HRTEM图像, 表面具有2 nm厚的连续且完全封闭的外壳[96]. (c) Pd@PtnL核壳结构纳米笼的高分辨HAADF-STEM图像[82]. (d) MoS2/Mo2C异质结构示意图[97]. (e) MoS2/Mo2C异质结构的高分辨率透射电镜图像[98]. (f) CNT@MoS2@C复合结构的HRTEM图像[99]. (g)等离子体辅助硒化工艺制备MoSe2/Mo核壳三维分级纳米结构的示意图. (h, i) FeCoNi复合纳米管阵列的SEM图像和元素分布[100], 比例尺分别为500 nm和200 nm

Figure 9. Open conformal structure of 2D materials. (a) Schematic of 2D MoS2-covered SiO2 microspheres[95]. (b) HRTEM images of Au/SiO2 nanoparticle with a continuous and completely packed shell with ca. 2 nm thickness[96]. (c) High-resolution HAADF-STEM image of a Pd@PtnL nanocage[82]. (d) Schematic of the MoS2/Mo2C heterostructure[97]. (e) High-resolution transmission electron microscopy (HRTEM) images of the MoS2/Mo2C heterostructure[98]. (f) HRTEM image of CNT@MoS2@C composite structure[99]. (g) Schematics of MoSe2/Mo core-shell 3D-hierarchical nanostructures prepared by the plasma-assisted selenization process. (h, i) Field-emission scanning electron microscope (SEM) images and EDX elemental mapping spectra of the as-prepared FeCoNi composite nanotubes. The scale bars are 500 and 200 nm, respectively[100]

图10. 二维材料的仿生共形结构. (a)石墨烯在硅藻基底表面生长及其仿生结构示意图[117]. (b)具有仿生结构的MoS2微观结构的TEM图像[118]. (c)具有猪笼草结构的石墨烯微观结构的TEM图像[119]. (d)由海胆脊柱合成的聚吡咯分层结构[120]. (e)以天然蟹壳为硬模板制备的有序介孔碳纳米纤维阵列[121]. (f)墨鱼骨表面CVD生长的仿生结构石墨烯, 插图为墨鱼骨照片[122]. (g)三维石墨烯泡沫制备过程示意图. (h)原始扇贝微观结构, (i)在空气中1050 ℃煅烧30 min后产物, (j) 1020 ℃下CVD生长石墨烯后产物, (k)刻蚀掉CaO后的贝壳状三维石墨烯泡沫[123]. 插图是相应的实物照片. 所有比例尺均为5 μm

Figure 10. Biomimetic structure of 2D materials. (a) Schematic of graphene growth on a diatom frustule and its hierarchical biomorphic structures[117]. (b) TEM image of the microstructure of the diatom frustule-derived MoS2[118]. (c) Nepenthes-like N-doped hierarchical graphene[119]. (d) Polypyrrole hierarchical architectures synthesized from a sea urchin spine[120]. (e) Highly ordered mesoporous carbon nanofiber arrays via a crab shell hard-templating synthetic process[121]. (f) CVD growth of graphene on cuttlebone substrates. The insert is top and bottom views of cuttlebones[122]. (g) Schematic illustration of Gr foam formation. SEM images of (h) pristine scallop microstructure, (i) Scallop calcined at 1050 ℃ for 30 min in air, (j) Calcined scallop after CVD graphene growth at 1020 ℃ for 30 min, (k) 3D graphene foam after removal of the CaO framework. Insets of panels h~k are the corresponding photographs[123]. All the scale bars are 5 μm

图11. 二维材料的人工有序微结构构筑. (a) PCF孔内壁CVD生长石墨烯的示意图. (b)石墨烯-PCF端面的SEM图像. (c)石墨烯-PCF端面的拉曼2D峰mapping图像. (d)从断裂的石墨烯-PCF的一个孔中伸出的管状石墨烯的SEM图像. (e)将石墨烯-PCF中刻蚀掉PCF之后留下的带有褶皱的石墨烯带的原子力显微镜(AFM)图像. 厚度约为2.0 nm[130]. (f) PCF和石墨烯-PCF的光学图像[131]. (g)注入浓度分别为1 mg?mL?1、4 mg?mL?1的Na2MoO4水溶液对所生长MoS2薄膜覆盖率的影响. (h)样品转移到微栅上之后, 管状的MoS2塌陷之后的STEM图像, 可以看到样品的质量很高, 晶体结构几乎没有缺陷[132]. (i)孔径内表面(孔径大小和PFC横截面都是微米级)完全被Graphene/hBN/Graphene薄膜完全覆盖(见右上角孔径内部放大示意图)的PCF结构示意图[133]

Figure 11. Artificial microstructures of 2D materials. (a) Schematics of graphene-PCF grown by the CVD method, with a graphene film on both the outer surface and inner walls of the PCF. (b) SEM image of the graphene-PCF end surface. (c) 2D-mode Raman intensity mapping of graphene at the fibre end surface. (d) SEM image of a tube-like graphene protruding out of one hole of the fractured graphene-PCF. (e) AFM image of a graphene ribbon with wrinkles. A height of ca. 2.0?nm is measured along the white dashed line[130]. (f) Transmission micrograph of bare PCF and graphene-PCF[131]. (g) Dependence of MoS2 coverage on the Na2MoO4 aqueous solution concentrations of 1 mg?mL?1, 4 mg?mL?1, respectively. (h) STEM image of collapsed tube-like MoS2 transferred onto a hollow grid, showing the high crystallinity of the as-grown MoS2 without detectable defects[132]. (i) The surface of air holes of PCF (hole diameter and pitch are both on the micron scale) is fully covered with Graphene/hBN/Graphene films (details in the top right panel)[133]

图12. 二维材料的复杂多孔结构. (a)双螺旋二十四面体结构介孔MoS2的合成方法及结构模型[140]. (b)三维石墨烯的SEM图像[141]. (c)三维MoS2的TEM图像[142]. (d)纳米多孔金基底上CVD制备单层MoS2@NPG工艺示意图[143]. (e) AMPSi@C(比例尺: 2 μm)的SEM图像[144]. (f) AMPSi@C的TEM图像(比例尺: 100 nm). 插图(比例尺: 10 nm)为HR-TEM图像, 显示在Si纳米微晶上包覆了5~8 nm厚度的非晶C壳层, 其晶格距离为0.31 nm, 对应于Si(111)晶面间距[144]. (g) 3D打印Ni泡沫溶解之前和溶解之后石墨烯泡沫的照片[145]. 比例尺为5 mm

Figure 12. Complex porous structures of 2D materials. (a) Synthesis procedure and structural model for mesoporous MoS2 with a double-gyroid (DG) morphology[140]. (b) SEM images of 3D graphene[141]. (c) TEM images of 3D MoS2[142]. (d) Schematic diagram of the fabrication process of MoS2@NPG hybrid materials by a nanoporous metal-based CVD approach[143]. (e) SEM image of AMPSi@C (scale bar: 2 μm)[144]. (f) TEM image of ant-nest-like microscale porous Si (AMPSi)@C (scale bar: 100 nm). The inset (scale bar: 10 nm) is the HRTEM image showing that the 5~8 nm thickness amorphous C shell is coated on the Si nanoligaments and the lattice distance of 0.31 nm corresponds to the d-spacing of the (111) planes of crystalline Si (111)[144]. (g) Photographs of 3D printed graphene foams before and after dissolving the Ni[145]. The scale bars are 5 mm

图13. 共形二维材料中光与物质的相互作用. (a) Au@SiO2在Pt(111)表面的模型. (b) Au@SiO2纳米颗粒的TEM图像. (c)经SHINs修饰的Pt (111)单晶电极表面的SEM图像. (d)基于Pt基底上2×2阵列模型的四个SHINs NPs的三维时域有限差分模拟. E和E0分别表示局域电场和入射电场[149]. (e) FGQF原理图. (f) FGQF的5/2缎面和缎织结构的SEM图像. (g) FGQF的屏蔽机理. (h)单根石墨烯-PCF (直径≈7 μm)的屏蔽机理, 以掺N石墨烯(黑色)包覆的PCF(黄色)为例[150]

Figure 13. The interaction between light and matter in conformal two-dimensional materials. (a) Model of shell-isolated nanoparticles (Au@SiO2 NPs, SHINs) at a Pt (111) surface. (b) TEM image of Au@SiO2 nanoparticles. (c) SEM image of a Pt (111) single-crystal electrode surface modified with SHINs. (d) 3D-FDTD simulations of four SHINs NPs with a model of a 2×2 array on a Pt substrate. E and E0 represent the localized electric field and the incident electric field, respectively[149]. (e) Schematics of FGQF. (f) SEM image of 5/2 satin and sateen weave structure of FGQF. (g) Shielding mechanisms of FGQF. (h) Shielding mechanisms of a single FM graphene quartz fiber (≈7 μm in diameter) as exemplified by quartz fiber (yellow) coated by graphitic N-doped Gr layers (black)[150]

图14. 光子晶体光纤. (a) HCF和MoS2-HCF的侧视光学图像. (b) MoS2-HCF的SHG光谱. (c) MoS2-HCF的THG光谱[132]. (d)基于石墨烯-PCF的电光调制器结构示意图. 通过石墨烯-PCF的光传输由离子溶液和石墨烯之间的栅极电压控制. (e)石墨烯-PCF调制器的传输调制(光纤长度归一化之后)的二维映射图, 入射光波长的函数与栅极电压的函数关系图. (f) 1310 nm和1550 nm波段处的调制曲线表明在“开启”和“关闭”状态之间有明确的转变, 且具有较大的调制深度[130]

Figure 14. Photonic crystal fiber. (a) Transmission micrograph of bare HCF and MoS2-HCF. SHG (b) and THG (c) spectra of MoS2-HCF[132]. (d) Schematic of a graphene-PCF-based electro-optic modulator. The gate voltage between the ionic liquid and graphene controls light transmission through the graphene-PCF. (e) 2D mapping of transmission modulation (normalized by fiber length) of the graphene-PCF modulator as a function of gate voltage and optical wavelength. (f) Modulation curves at 1310 and 1550?nm show an unambiguous transition between the ‘on’ and ‘off’ state with large modulation depth[130]

图15. 二维材料表面修饰的电极. (a) MoS2@NPG结构示意图. (b) Au基底上单层MoS2@NPG的高分辨率STEM图像和2H MoS2结构模型的模拟STEM图像. (c, d)显示MoS2@NPG起始电位和相应的Tafel斜率的电极极化曲线[143]. (e) MnO纳米棒上石墨烯笼状结构生长示意图. (f)在扫描速率为50 μV?s?1时, MnO@多层缺陷石墨烯电极与Li/Li+在0.01~3 V电位窗口内的循环伏安曲线. (g) MnO@多层缺陷石墨烯电极与纯MnO电极的长循环性能比较. 倍率分别为0.05 C(3次循环)和0.15 C(200次循环)[167]

Figure 15. Surface modification of electrodes. (a) Schematic of the monolayer MoS2@NPG. (b) Higher resolution STEM images of monolayer MoS2@NPG from the flat region of a gold ligament. The inset shows the simulated STEM image based on the standard structure model of 2H MoS2. (c, d) Derivative polarization curves showing the onset potentials and corresponding Tafel slopes of MoS2@NPG[143]. (e) Schematic diagram of the growth of graphene cage-like structure on MnO nanorods. (f) Cyclic voltammetry curves of the MnO@defected graphene electrodes in a potential window of 0.01~3 V versus Li/Li+ collected at a scan rate of 50 μV?s?1. (g) Long-term electrochemical cycling of MnO@MDFG electrode compared with the bare MnO electrode. The rate is 0.05 C for 3 cycles and 0.15 C for 200 cycles, respectively[167]

图16. 共形二维材料的多样化应用. (a) CNT@Si@C颗粒在不同锂化状态下(比例尺: 0.5 μm). (b) (a)中CNT@Si@C颗粒在锂化过程中的体积膨胀曲线[169]. (c)金属氧化物三维共形结构过滤水的示意图与光学图像[170]. 12 d (d)和6 h (e)内DOPA/氧化铁修饰硅藻土对吲哚美辛的释放效率, 插图为载药后样品SEM图像[111]. (f)暴露于NO气氛(3、5或8 cm3/m3浓度)下器件的电流(I)响应曲线. 数据每秒收集一次. 插图是附着在两个铂电极上的SnO2共形涂覆硅藻土结构的SEM图像[171]

Figure 16. Various applications of conformal 2D materials. (a) In-situ TEM images of a CNT@Si@C particle at different lithiation states (scale bar: 0.5 μm). (b) Volume expansion curve of the particle recorded during the lithiation process[169]. (c) Optical image of the filter and a schematic description of the filtration process[170]. (d, e) The drug release of indomethacin from DOPA/iron oxide modified diatoms over (d) 12 d and (e) 6 h. The insert is SEM image of surface after drug loading[111]. (f) Current (I) response upon exposure to NO gas (3, 5, or 8 cm3/m3 in argon). The insert is SEM of the SnO2-coated valves attached to two platinum electrodes[171]

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共形二维材料: 创制与应用

Conformal Two-Dimensional Materials: Preparation and Applications

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