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Title: Hierarchical Nanoassembly of MoS{sub 2}/Co{sub 9}S{sub 8}/Ni{sub 3}S{sub 2}/Ni as a Highly Efficient Electrocatalyst for Overall Water Splitting in a Wide pH Range.

Abstract

The design of low-cost yet high-efficiency electrocatalysts for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) over a wide pH range is highly challenging. We now report a hierarchical co-assembly of interacting MoS2 and Co9S8 nanosheets attached on Ni3S2 nanorod arrays which are supported on nickel foam (NF). This tiered structure endows high performance toward HER and OER over a very broad pH range. By adjusting the molar ratio of the Co:Mo precursors, we have created CoMoNiS-NF-xy composites (x:y means Co:Mo molar ratios ranging from 5:1 to 1:3) with controllable morphology and composition. The three-dimensional composites have an abundance of active sites capable of universal pH catalytic HER and OER activity. The CoMoNiS-NF-31 demonstrates the best electrocatalytic activity, giving ultralow overpotentials (113, 103, and 117 mV for HER and 166, 228, and 405 mV for OER) to achieve a current density of 10 mA cm(-2) in alkaline, acidic, and electrolytes, respectively. It also shows a remarkable balance between electrocatalytic activity and stability. Based on the distinguished catalytic performance of CoMoNiS-NF-31 toward HER and OER, we demonstrate a two-electrode electrolyzer performing water electrolysis over a wide pH range, with low cell voltages of 1.54, 1.45, and 1.80 V at 10more » mA cm(-2) in alkaline, acidic, and neutral media, respectively. First-principles calculations suggest that the high OER activity arises from electron transfer from Co9S8 to MoS2 at the interface, which alters the binding energies of adsorbed species and decreases overpotentials. Our results demonstrate that hierarchical metal sulfides can serve as highly efficient all-pH (pH = 0-14) electrocatalysts for overall water splitting.« less

Authors:
; ; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
National Science Foundation of China; USDOE Office of Science - Office of Basic Energy Sciences - Materials Sciences and Engineering Division
OSTI Identifier:
1545600
DOE Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 141; Journal Issue: 26
Country of Publication:
United States
Language:
English

Citation Formats

Yang, Yan, Yao, Huiqin, Yu, Zihuan, Islam, Saiful M., He, Haiying, Yuan, Mengwei, Yue, Yonghai, Xu, Kang, Hao, Weichang, Sun, Genban, Zapol, Peter, and Kanatzidis, Mercouri G. Hierarchical Nanoassembly of MoS{sub 2}/Co{sub 9}S{sub 8}/Ni{sub 3}S{sub 2}/Ni as a Highly Efficient Electrocatalyst for Overall Water Splitting in a Wide pH Range.. United States: N. p., 2019. Web. doi:10.1021/jacs.9b04492.
Yang, Yan, Yao, Huiqin, Yu, Zihuan, Islam, Saiful M., He, Haiying, Yuan, Mengwei, Yue, Yonghai, Xu, Kang, Hao, Weichang, Sun, Genban, Zapol, Peter, & Kanatzidis, Mercouri G. Hierarchical Nanoassembly of MoS{sub 2}/Co{sub 9}S{sub 8}/Ni{sub 3}S{sub 2}/Ni as a Highly Efficient Electrocatalyst for Overall Water Splitting in a Wide pH Range.. United States. doi:10.1021/jacs.9b04492.
Yang, Yan, Yao, Huiqin, Yu, Zihuan, Islam, Saiful M., He, Haiying, Yuan, Mengwei, Yue, Yonghai, Xu, Kang, Hao, Weichang, Sun, Genban, Zapol, Peter, and Kanatzidis, Mercouri G. Wed . "Hierarchical Nanoassembly of MoS{sub 2}/Co{sub 9}S{sub 8}/Ni{sub 3}S{sub 2}/Ni as a Highly Efficient Electrocatalyst for Overall Water Splitting in a Wide pH Range.". United States. doi:10.1021/jacs.9b04492.
@article{osti_1545600,
title = {Hierarchical Nanoassembly of MoS{sub 2}/Co{sub 9}S{sub 8}/Ni{sub 3}S{sub 2}/Ni as a Highly Efficient Electrocatalyst for Overall Water Splitting in a Wide pH Range.},
author = {Yang, Yan and Yao, Huiqin and Yu, Zihuan and Islam, Saiful M. and He, Haiying and Yuan, Mengwei and Yue, Yonghai and Xu, Kang and Hao, Weichang and Sun, Genban and Zapol, Peter and Kanatzidis, Mercouri G.},
abstractNote = {The design of low-cost yet high-efficiency electrocatalysts for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) over a wide pH range is highly challenging. We now report a hierarchical co-assembly of interacting MoS2 and Co9S8 nanosheets attached on Ni3S2 nanorod arrays which are supported on nickel foam (NF). This tiered structure endows high performance toward HER and OER over a very broad pH range. By adjusting the molar ratio of the Co:Mo precursors, we have created CoMoNiS-NF-xy composites (x:y means Co:Mo molar ratios ranging from 5:1 to 1:3) with controllable morphology and composition. The three-dimensional composites have an abundance of active sites capable of universal pH catalytic HER and OER activity. The CoMoNiS-NF-31 demonstrates the best electrocatalytic activity, giving ultralow overpotentials (113, 103, and 117 mV for HER and 166, 228, and 405 mV for OER) to achieve a current density of 10 mA cm(-2) in alkaline, acidic, and electrolytes, respectively. It also shows a remarkable balance between electrocatalytic activity and stability. Based on the distinguished catalytic performance of CoMoNiS-NF-31 toward HER and OER, we demonstrate a two-electrode electrolyzer performing water electrolysis over a wide pH range, with low cell voltages of 1.54, 1.45, and 1.80 V at 10 mA cm(-2) in alkaline, acidic, and neutral media, respectively. First-principles calculations suggest that the high OER activity arises from electron transfer from Co9S8 to MoS2 at the interface, which alters the binding energies of adsorbed species and decreases overpotentials. Our results demonstrate that hierarchical metal sulfides can serve as highly efficient all-pH (pH = 0-14) electrocatalysts for overall water splitting.},
doi = {10.1021/jacs.9b04492},
journal = {Journal of the American Chemical Society},
number = 26,
volume = 141,
place = {United States},
year = {2019},
month = {7}
}