Modulation of Water Dissociation Kinetics with a "Breathable" Wooden Electrode for Efficient Hydrogen Evolution

ACS Appl Mater Interfaces. 2022 Feb 9;14(5):6818-6827. doi: 10.1021/acsami.1c22601. Epub 2022 Jan 25.

Abstract

Innovative breakthroughs regarding self-supported open and porous electrodes that can promote gas-liquid transmission and regulate the water dissociation kinetics are critical for sustainable hydrogen economy. Herein, a free-standing porous electrode with Pd-NiS nanoparticles assembled in a multichannel carbonized wood framework (Pd-NiS/CW) was ingeniously constructed. Specifically, carbonized wood (CW) with a mass of open microchannels and high electrical conductivity can significantly facilitate electrolyte permeation ("inhalation"), hydrogen evolution ("exhalation"), and electron transfer. As expected, the fabricated "breathable" wooden electrode exhibits remarkable hydrogen evolution activity in 1.0 M KOH, only requiring a low overpotential of 80 mV to sustain a current density of 10 mA cm-2, and can maintain this current density for 100 h. Further, the spectroscopic characterization and density functional theory (DFT) calculations manifest that the electron interaction between Pd and NiS is beneficial to reduce the water dissociation energy barriers, optimize the adsorption/desorption of H, and ultimately accelerate the catalytic activity. The work reported here will provide a potential approach for the design of electrocatalysts combined with natural multichannel wood to achieve the goal of high electrocatalytic activity and superior durability for hydrogen production.

Keywords: Pd-NiS composite catalyst; carbonized wood framework; hydrogen evolution reaction; water dissociation kinetics; “breathable”.