Ambipolar Electrochemistry of Pre‐Intercalated Ti 3 C 2 T x MXene in Ionic Liquid Electrolyte

Valurouthu, Geetha; Panigrahi, Rachita; Saraf, Mohit; Shuck, Christopher E.; Mallik, Bhabani S.; Kurra, Narendra; Gogotsi, Yury

doi:10.1002/batt.202300009

Ambipolar Electrochemistry of Pre‐Intercalated Ti ₃ C ₂ T _x MXene in Ionic Liquid Electrolyte

Journal Article · Mon Mar 20 04:00:00 EDT 2023 · Batteries & Supercaps

DOI:https://doi.org/10.1002/batt.202300009· OSTI ID:2422595

Valurouthu, Geetha ^[1]; Panigrahi, Rachita ^[2]; ^[1]; Shuck, Christopher E. ^[1]; Mallik, Bhabani S. ^[2]; Kurra, Narendra ^[2]; ^[1]

A. J. Drexel Nanomaterials Institute and Department of Materials Science and Engineering Drexel University Philadelphia PA 19104 USA
Department of Chemistry Indian Institute of Technology Hyderabad Kandi 502284, Sangareddy Telangana State India

Abstract

Cation intercalation with or without redox remains the dominant charge storage mechanism for two‐dimensional (2D) Ti₃C₂T_xMXene. Anion‐based charge storage remains unexplored due to intrinsic negative surface charge of MXenes preventing spontaneous intercalation of anions and irreversible oxidation of Ti at anodic potentials in aqueous electrolytes. In this work, we report on the ambipolar electrochemical behavior of the Ti₃C₂T_xin ionic liquid electrolyte over a 2.5 V electrochemically stable window. The experiments are conducted on a thin Ti₃C₂T_xfilm current collector coated with an electroactive layer of small flakes (∼150 nm) of Ti₃C₂T_xpre‐intercalated with 1‐ethyl‐3‐methylimidazolium bis‐(trifluoromethylsulfonyl)‐imide (EMIM‐TFSI) ionic liquid. Couples of redox peaks with a very small potential separation during the voltage sweep are observed at high negative (−0.75 V vs. Ag wire) and high positive (+0.75 V vs. Ag wire) potentials. Our experimental electrochemical data combined with density functional theory (DFT) calculations suggest feasibility of pseudo‐intercalation of TFSI anions between Ti₃C₂T_xflakes. This study provides a pathway for elucidating anion intercalation for different MXene chemistries in solvent‐free electrolytes, which can lead to development of MXene based energy storage devices with improved performance.

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Fluid Interface Reactions, Structures and Transport Center (FIRST)

Sponsoring Organization:: USDOE

DOE Contract Number:: AC02-05CH11231

OSTI ID:: 2422595

Journal Information:: Batteries & Supercaps, Journal Name: Batteries & Supercaps Journal Issue: 5 Vol. 6; ISSN 2566-6223

Publisher:: Wiley

Country of Publication:: United States

Language:: English

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