TY - JOUR
T1 - Facilitated Water Adsorption and Dissociation on Ni/Ni3S2 Nanoparticles Embedded in Porous S-doped Carbon Nanosheet Arrays for Enhanced Hydrogen Evolution
AU - Li, Yong
AU - Patel, Dipam M.
AU - Tsang, Chui Shan
AU - Zhang, Renqin
AU - Liu, Mengjie
AU - Hwang, Gyeong S.
AU - Lee, Lawrence Yoon Suk
N1 - Funding Information:
This work was supported by the Innovation and Technology Commission of Hong Kong and Hong Kong Polytechnic University (1‐BE0Y). G.S.H. gratefully acknowledges the support of the R.A. Welch Foundation (F‐1535). The authors also thank Myungsuk Lee and Bohak Yoon in the Hwang group for sharing their simulation results on the arrangement and dynamics of water at the catalyst/water interface as well as the Texas Advanced Computing Center for use of the Stampede supercomputing system (OCI‐1134872).
Publisher Copyright:
© 2020 Wiley-VCH GmbH
Copyright:
Copyright 2020 Elsevier B.V., All rights reserved.
PY - 2020
Y1 - 2020
N2 - Three-dimensional carbon-based catalysts grown on a conductive substrate offer superior electrocatalytic activities toward hydrogen evolution reaction (HER). Herein, a novel method is described for in situ fabrication of hybrid Ni/Ni3S2 nanoparticles embedded in S-doped carbon nanosheet arrays (Ni/Ni3S2/SC NSAs) on carbon cloth. With the morphological merits of large surface area and high conductivity, Ni/Ni3S2/SC NSAs are demonstrated as an efficient and durable HER catalyst that requires merely 90 mV at a current density of 10 mA cm−2 with a small Tafel slope of 81 mV dec−1. This excellent performance is ascribed to the excellent H2O adsorption property of S-doped C layer and formation of Niδ+ and Sδ− species that promote the cleavage of H–OH bonds. First-principles calculations further reveal that the Ni surface near the Ni/Ni3S2 interface has a larger water adsorption energy (Ead) and lower activation energy for water dissociation (Ea) than pure Ni and Ni3S2, which contribute to enhanced HER performance. This work offers valuable insights into the designing of interface between transition metal-based catalysts and heteroatom-doped carbon materials.
AB - Three-dimensional carbon-based catalysts grown on a conductive substrate offer superior electrocatalytic activities toward hydrogen evolution reaction (HER). Herein, a novel method is described for in situ fabrication of hybrid Ni/Ni3S2 nanoparticles embedded in S-doped carbon nanosheet arrays (Ni/Ni3S2/SC NSAs) on carbon cloth. With the morphological merits of large surface area and high conductivity, Ni/Ni3S2/SC NSAs are demonstrated as an efficient and durable HER catalyst that requires merely 90 mV at a current density of 10 mA cm−2 with a small Tafel slope of 81 mV dec−1. This excellent performance is ascribed to the excellent H2O adsorption property of S-doped C layer and formation of Niδ+ and Sδ− species that promote the cleavage of H–OH bonds. First-principles calculations further reveal that the Ni surface near the Ni/Ni3S2 interface has a larger water adsorption energy (Ead) and lower activation energy for water dissociation (Ea) than pure Ni and Ni3S2, which contribute to enhanced HER performance. This work offers valuable insights into the designing of interface between transition metal-based catalysts and heteroatom-doped carbon materials.
KW - electrocatalytic hydrogen evolution
KW - electronic interaction
KW - Ni/Ni S hybrid nanoparticles
KW - S-doped carbon nanosheets
UR - http://www.scopus.com/inward/record.url?scp=85096765092&partnerID=8YFLogxK
U2 - 10.1002/admi.202001665
DO - 10.1002/admi.202001665
M3 - Journal article
AN - SCOPUS:85096765092
SN - 2196-7350
VL - 8
JO - Advanced Materials Interfaces
JF - Advanced Materials Interfaces
IS - 1
M1 - 2001665
ER -