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Research Article

Electrostatically connected nanoarchitected electrocatalytic films for boosted water splitting

Chao-Peng Wang1,§, Hao Sun1,§, Gang Bian1, Jia-Xi Wang1, Xixi Pang1, Guoqi Wang1, Jian Zhu1,2,3( ), Xian-He Bu1,2( )
School of Materials Science and Engineering, National Institute for Advanced Materials, Nankai University, Tianjin 300350, China
Tianjin Key Laboratory of Metal and Molecule-Based Material Chemistry, Nankai University, Tianjin 300350, China
Tianjin Key Laboratory for Rare Earth Materials and Applications, Nankai University, Tianjin 300350, China

§ Chao-Peng Wang and Hao Sun contributed equally to this work.

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Graphical Abstract

Ultrathin two-dimensional (2D) electrocatalysts with ordered stacking and controllable thicknesses can be homogeneously deposited via layer-by-layer (LbL) assembly on desired surfaces with enhanced water splitting performance. Such nanofilms can possess high mass activities, which are ~ 20 times those of drop-casted films.

Abstract

Active sites of two-dimensional (2D) electrocatalysts are often partially blocked owing to their inevitable stacking and hydrophobic polymeric binders in macroscale electrodes, therefore impeding their applications in efficient electrolyzers. Here, using layered double hydroxide (LDH) nanosheets as a model 2D electrocatalyst, we demonstrate that their performance toward water splitting can be boosted when they are electrostatically assembled into an organized structure pillared by hydrophilic polyelectrolytes or nanoparticles in a layer-by-layer (LbL) fashion. In particular, their mass activity on a planar electrode can be as large as 2.267 mA·μg−1 toward oxygen evolution reaction (OER), when NiFe-LDH nanosheets are electrostatically connected by poly(sodium 4-styrenesulfonate) (PSS), while drop-casted NiFe-LDH nanosheets only have a mass activity of 0.116 mA·μg−1. In addition, these homogeneous NiFe-LDH nanofilms can be easily deposited on three-dimensional (3D) surfaces with high areas, such as carbon cloths, to serve as practical electrodes with overpotentials of 328 mV at a current density of 100 mA·cm−2, and stability for 40 h. Furthermore, Pt nanoparticles can be LbL assembled with NiFe-LDH as bifunctional electrodes for synergistically boosted oxygen and hydrogen evolution reactions (HER), leading to successful overall water splitting powered by a 1.5 V battery. This study heralds the spatial control of 2D nanomaterials in nanoscale precision as an efficient strategy for the design of advanced electrocatalysts.

Keywords

layer-by-layer (LbL) assemblylayered double hydroxides (LDH)two-dimensional (2D) electrocatalystsoxygen evolution reaction (OER)water splitting

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Nano Research
Volume 17 Issue 3,
March 2024
Pages 1114-1122
DOI: 10.1007/s12274-023-5917-2
Cite this article:
Wang C-P, Sun H, Bian G, et al. Electrostatically connected nanoarchitected electrocatalytic films for boosted water splitting. Nano Research, 2024, 17(3): 1114-1122. https://doi.org/10.1007/s12274-023-5917-2
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Received: 27 April 2023
Revised: 31 May 2023
Accepted: 11 June 2023
Published: 01 August 2023
© Tsinghua University Press 2023
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