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Hierarchically Porous 3D Freestanding Holey-MXene Framework via Mild Oxidation of Self-Assembled MXene Hydrogel for Ultrafast Pseudocapacitive Energy Storage

Sikdar, Anirban ; Héraly, Frédéric ; Zhang, Hao ; Hall, Stephen LU ; Pang, Kanglei ; Zhang, Miao and Yuan, Jiayin (2024) In ACS Nano 18(4). p.3707-3719
Abstract

The true promise of MXene as a practical supercapacitor electrode hinges on the simultaneous advancement of its three-dimensional (3D) assembly and the engineering of its nanoscopic architecture, two critical factors for facilitating mass transport and enhancing an electrode’s charge-storage performance. Herein, we present a straightforward strategy to engineer robust 3D freestanding MXene (Ti3C2Tx) hydrogels with hierarchically porous structures. The tetraamminezinc(II) complex cation ([Zn(NH3)4]2+) is selected to electrostatically assemble colloidal MXene nanosheets into a 3D interconnected hydrogel framework, followed by a mild oxidative acid-etching process to create... (More)

The true promise of MXene as a practical supercapacitor electrode hinges on the simultaneous advancement of its three-dimensional (3D) assembly and the engineering of its nanoscopic architecture, two critical factors for facilitating mass transport and enhancing an electrode’s charge-storage performance. Herein, we present a straightforward strategy to engineer robust 3D freestanding MXene (Ti3C2Tx) hydrogels with hierarchically porous structures. The tetraamminezinc(II) complex cation ([Zn(NH3)4]2+) is selected to electrostatically assemble colloidal MXene nanosheets into a 3D interconnected hydrogel framework, followed by a mild oxidative acid-etching process to create nanoholes on the MXene surface. These hierarchically porous, conductive holey-MXene frameworks facilitate 3D transport of both electrons and electrolyte ions to deliver an excellent specific capacitance of 359.2 F g-1 at 10 mV s-1 and superb capacitance retention of 79% at 5000 mV s-1, representing a 42.2% and 15.3% improvement over pristine MXene hydrogel, respectively. Even at a commercial-standard mass loading of 10.1 mg cm-2, it maintains an impressive capacitance retention of 52% at 1000 mV s-1. This rational design of an electrode by engineering nanoholes on MXene nanosheets within a 3D porous framework dictates a significant step forward toward the practical use of MXene and other 2D materials in electrochemical energy storage systems.

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author
; ; ; ; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
2D materials, freestanding hydrogel, holey-MXene, pseudocapacitor, self-assembly
in
ACS Nano
volume
18
issue
4
pages
13 pages
publisher
The American Chemical Society (ACS)
external identifiers
  • scopus:85183528105
  • pmid:38230678
ISSN
1936-0851
DOI
10.1021/acsnano.3c11551
language
English
LU publication?
yes
id
7dffa2b5-0026-4948-8ee1-ac224e09cc6d
date added to LUP
2024-02-15 15:33:30
date last changed
2025-02-05 20:40:43
@article{7dffa2b5-0026-4948-8ee1-ac224e09cc6d,
  abstract     = {{<p>The true promise of MXene as a practical supercapacitor electrode hinges on the simultaneous advancement of its three-dimensional (3D) assembly and the engineering of its nanoscopic architecture, two critical factors for facilitating mass transport and enhancing an electrode’s charge-storage performance. Herein, we present a straightforward strategy to engineer robust 3D freestanding MXene (Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub>) hydrogels with hierarchically porous structures. The tetraamminezinc(II) complex cation ([Zn(NH<sub>3</sub>)<sub>4</sub>]<sup>2+</sup>) is selected to electrostatically assemble colloidal MXene nanosheets into a 3D interconnected hydrogel framework, followed by a mild oxidative acid-etching process to create nanoholes on the MXene surface. These hierarchically porous, conductive holey-MXene frameworks facilitate 3D transport of both electrons and electrolyte ions to deliver an excellent specific capacitance of 359.2 F g<sup>-1</sup> at 10 mV s<sup>-1</sup> and superb capacitance retention of 79% at 5000 mV s<sup>-1</sup>, representing a 42.2% and 15.3% improvement over pristine MXene hydrogel, respectively. Even at a commercial-standard mass loading of 10.1 mg cm<sup>-2</sup>, it maintains an impressive capacitance retention of 52% at 1000 mV s<sup>-1</sup>. This rational design of an electrode by engineering nanoholes on MXene nanosheets within a 3D porous framework dictates a significant step forward toward the practical use of MXene and other 2D materials in electrochemical energy storage systems.</p>}},
  author       = {{Sikdar, Anirban and Héraly, Frédéric and Zhang, Hao and Hall, Stephen and Pang, Kanglei and Zhang, Miao and Yuan, Jiayin}},
  issn         = {{1936-0851}},
  keywords     = {{2D materials; freestanding hydrogel; holey-MXene; pseudocapacitor; self-assembly}},
  language     = {{eng}},
  number       = {{4}},
  pages        = {{3707--3719}},
  publisher    = {{The American Chemical Society (ACS)}},
  series       = {{ACS Nano}},
  title        = {{Hierarchically Porous 3D Freestanding Holey-MXene Framework via Mild Oxidation of Self-Assembled MXene Hydrogel for Ultrafast Pseudocapacitive Energy Storage}},
  url          = {{http://dx.doi.org/10.1021/acsnano.3c11551}},
  doi          = {{10.1021/acsnano.3c11551}},
  volume       = {{18}},
  year         = {{2024}},
}