Ultrasonic-Ball Milling: A Novel Strategy to Prepare Large-Size Ultrathin 2D Materials.

Large-size ultrathin 2D materials, with extensive applications in optics, medicine, biology, and semiconductor fields, can be prepared through an existing common physical and chemical process. However, the current exfoliation technologies still need to be improved upon with urgency. Herein, a novel and simple "ultrasonic-ball milling" strategy is reported to effectively obtain high quality and large size ultrathin 2D materials with complete lattice structure through the introduction of moderate sapphire (Al2 O3 ) abrasives in a liquid phase system. Ultimately numerous high-quality ultrathin h-BN, graphene, MoS2 , WS2 , and BCN nanosheets are obtained with large sizes ranging from 1-20 µm, small thickness of ≈1-3 nm and a high yield of over 20%. Utilizing shear and friction force synergistically, this strategy provides a new method and alternative for preparing and optimizing large size ultrathin 2D materials.

[1]  Jianlin Shi,et al.  Silicene: Wet‐Chemical Exfoliation Synthesis and Biodegradable Tumor Nanomedicine , 2019, Advanced materials.

[2]  Xun Wang,et al.  Metallic Transition-Metal Dichalcogenide Nanocatalysts for Energy Conversion , 2018, Chem.

[3]  Timothy C. Berkelbach,et al.  Many-body simulation of two-dimensional electronic spectroscopy of excitons and trions in monolayer transition metal dichalcogenides , 2018, Nature Communications.

[4]  U. Waghmare,et al.  Superior performance of borocarbonitrides, BxCyNz, as stable, low-cost metal-free electrocatalysts for the hydrogen evolution reaction , 2016 .

[5]  Shouzhi Wang,et al.  Band gap-Tunable Porous Borocarbonitride Nanosheets for High Energy-Density Supercapacitors. , 2018, ACS applied materials & interfaces.

[6]  K. Amine,et al.  1T MoS2 nanosheets with extraordinary sodium storage properties via thermal-driven ion intercalation assisted exfoliation of bulky MoS2 , 2019, Nano Energy.

[7]  Hua Zhang Ultrathin Two-Dimensional Nanomaterials. , 2015, ACS nano.

[8]  Q. Fu,et al.  Epitaxial Growth of h‐BN on Templates of Various Dimensionalities in h‐BN–Graphene Material Systems , 2019, Advanced materials.

[9]  Hugen Yan,et al.  Anomalous lattice vibrations of single- and few-layer MoS2. , 2010, ACS nano.

[10]  Song Gao,et al.  A Universal Strategy for Hollow Metal Oxide Nanoparticles Encapsulated into B/N Co‐Doped Graphitic Nanotubes as High‐Performance Lithium‐Ion Battery Anodes , 2018, Advanced materials.

[11]  Yunhui Huang,et al.  Exploring Sodium-Ion Storage Mechanism in Hard Carbons with Different Microstructure Prepared by Ball-Milling Method. , 2018, Small.

[12]  S. Komarneni,et al.  An in situ anion exchange induced high-performance oxygen evolution reaction catalyst for the pH-near-neutral potassium borate electrolyte , 2019, Journal of Materials Chemistry A.

[13]  A. Sinitskii,et al.  Quasi-1D TiS3 Nanoribbons: Mechanical Exfoliation and Thickness-Dependent Raman Spectroscopy. , 2018, ACS nano.

[14]  A. Govindaraj,et al.  Supercapacitors based on composites of PANI with nanosheets of nitrogen-doped RGO, BC1.5N, MoS2 and WS2 , 2015 .

[15]  N. Peres,et al.  1 Universal Dynamic Conductivity and Quantized Visible Opacity of Suspended Graphene , 2008 .

[16]  Gang Zhao,et al.  Fabrication of two-dimensional nanosheets via water freezing expansion exfoliation , 2014, Nanotechnology.

[17]  J. Shan,et al.  Photonics and optoelectronics of 2D semiconductor transition metal dichalcogenides , 2016, Nature Photonics.

[18]  Hua Zhang,et al.  The chemistry of two-dimensional layered transition metal dichalcogenide nanosheets. , 2013, Nature chemistry.

[19]  Andre K. Geim,et al.  The rise of graphene. , 2007, Nature materials.

[20]  Aaron M. Jones,et al.  Virtual Trions in the Photoluminescence of Monolayer Transition-Metal Dichalcogenides. , 2018, Physical review letters.

[21]  S. Pennycook,et al.  From Self‐Assembly Hierarchical h‐BN Patterns to Centimeter‐Scale Uniform Monolayer h‐BN Film , 2018, Advanced Materials Interfaces.

[22]  H. Zeng,et al.  Single-Layered MoS2 Directly Grown on Rutile TiO2(110) for Enhanced Interfacial Charge Transfer. , 2019, ACS nano.

[23]  Andre K. Geim,et al.  Electric Field Effect in Atomically Thin Carbon Films , 2004, Science.

[24]  M. Chhetri,et al.  Borocarbonitrides as Metal‐Free Catalysts for the Hydrogen Evolution Reaction , 2018, Advanced materials.

[25]  C. Rao,et al.  Borocarbonitrides, BxCyNz: Synthesis, Characterization, and Properties with Potential Applications. , 2017, ACS applied materials & interfaces.

[26]  Hua Zhang,et al.  High phase-purity 1T′-MoS2- and 1T′-MoSe2-layered crystals , 2018, Nature Chemistry.

[27]  A. Bostwick,et al.  Giant spin-splitting and gap renormalization driven by trions in single-layer WS2/h-BN heterostructures , 2017, 1705.04866.

[28]  Junle Qu,et al.  Ultrathin 2D Nonlayered Tellurium Nanosheets: Facile Liquid‐Phase Exfoliation, Characterization, and Photoresponse with High Performance and Enhanced Stability , 2018 .

[29]  J. Llorca,et al.  Outstanding Methane Oxidation Performance of Palladium-Embedded Ceria Catalysts Prepared by a One-Step Dry Ball-Milling Method. , 2018, Angewandte Chemie.

[30]  Jack C. Lee,et al.  Thinnest Nonvolatile Memory Based on Monolayer h‐BN , 2019, Advanced materials.

[31]  Dominique Baillargeat,et al.  From Bulk to Monolayer MoS2: Evolution of Raman Scattering , 2012 .

[32]  Gang Zhao,et al.  Large-quantity and continuous preparation of two-dimensional nanosheets. , 2016, Nanoscale.

[33]  A. Kis,et al.  Electronic Properties of Transferable Atomically Thin MoSe2/h-BN Heterostructures Grown on Rh(111). , 2018, ACS nano.

[34]  J. Shan,et al.  Atomically thin MoS₂: a new direct-gap semiconductor. , 2010, Physical review letters.

[35]  Yongzhong Wu,et al.  A facile chemical exfoliation method to obtain large size boron nitride nanosheets , 2013 .

[36]  K. Müllen,et al.  Exfoliation of graphite into graphene in aqueous solutions of inorganic salts. , 2014, Journal of the American Chemical Society.

[37]  Hui-Ming Cheng,et al.  Chemical Vapor Deposition Growth and Applications of Two-Dimensional Materials and Their Heterostructures. , 2018, Chemical reviews.

[38]  R. Schloegl,et al.  A Peeling Approach for Integrated Manufacturing of Large Monolayer h-BN Crystals. , 2018, ACS nano.