Direct Fabrication of Atomically Defined Pores in MXenes Using Feedback‐Driven STEM

Author:

Boebinger Matthew G.1ORCID,Yilmaz Dundar E.2,Ghosh Ayana3ORCID,Misra Sudhajit1ORCID,Mathis Tyler S.4ORCID,Kalinin Sergei V.5ORCID,Jesse Stephen1ORCID,Gogotsi Yury4ORCID,van Duin Adri C. T.2ORCID,Unocic Raymond R.1ORCID

Affiliation:

1. Center for Nanophase Materials Sciences Oak Ridge National Laboratory Oak Ridge TN 37831 USA

2. Department of Mechanical Engineering The Pennsylvania State University University Park PA 16802 USA

3. Computational Sciences and Engineering Division Oak Ridge National Laboratory Oak Ridge TN 37831 USA

4. A.J. Drexel Nanomaterials Institute and Department of Materials Science and Engineering Drexel University Philadelphia PA 19104 USA

5. Department of Materials Science and Engineering University of Tennessee Knoxville TN 37996 USA

Abstract

AbstractControlled fabrication of nanopores in 2D materials offer the means to create robust membranes needed for ion transport and nanofiltration. Techniques for creating nanopores have relied upon either plasma etching or direct irradiation; however, aberration‐corrected scanning transmission electron microscopy (STEM) offers the advantage of combining a sub‐Å sized electron beam for atomic manipulation along with atomic resolution imaging. Here, a method for automated nanopore fabrication is utilized with real‐time atomic visualization to enhance the mechanistic understanding of beam‐induced transformations. Additionally, an electron beam simulation technique, Electron‐Beam Simulator (E‐BeamSim) is developed to observe the atomic movements and interactions resulting from electron beam irradiation. Using the MXene Ti3C2Tx, the influence of temperature on nanopore fabrication is explored by tracking atomic transformations and find that at room temperature the electron beam irradiation induces random displacement and results in titanium pileups at the nanopore edge, which is confirmed by E‐BeamSim. At elevated temperatures, after removal of the surface functional groups and with the increased mobility of atoms results in atomic transformations that lead to the selective removal of atoms layer by layer. This work can lead to the development of defect engineering techniques within functionalized MXene layers and other 2D materials.

Funder

U.S. Department of Energy

Basic Energy Sciences

Energy Frontier Research Centers

National Science Foundation

Publisher

Wiley

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