Engineering monolayer 1T-MoS2 into a bifunctional electrocatalyst via sonochemical doping of isolated transition metal atoms

There has been an intense research effort to develop 2-H MoS2 based catalysts to reduce or eliminate the use of Pt/C at higher metal loading for the hydrogen evolution reaction (HER) in catalytic hydrolysis of water, which enables the capture of renewable energy sources as fuel and chemical. However...

Full description

Bibliographic Details
Main Authors: Lau, THM, Wu, S, Kato, R, Wu, T-S, Kulhavy, J, Mo, J, Zheng, J, Foord, JS, Soo, Y-L, Suenaga, K, Darby, MT, Tsang, SCE
Format: Journal article
Language:English
Published: American Chemical Society 2019
_version_ 1797075736246353920
author Lau, THM
Wu, S
Kato, R
Wu, T-S
Kulhavy, J
Mo, J
Zheng, J
Foord, JS
Soo, Y-L
Suenaga, K
Darby, MT
Tsang, SCE
author_facet Lau, THM
Wu, S
Kato, R
Wu, T-S
Kulhavy, J
Mo, J
Zheng, J
Foord, JS
Soo, Y-L
Suenaga, K
Darby, MT
Tsang, SCE
author_sort Lau, THM
collection OXFORD
description There has been an intense research effort to develop 2-H MoS2 based catalysts to reduce or eliminate the use of Pt/C at higher metal loading for the hydrogen evolution reaction (HER) in catalytic hydrolysis of water, which enables the capture of renewable energy sources as fuel and chemical. However, the study of its uncommon polymorph, 1T-MoS2, and particularly the doping effect with transition metal (TM) is rather limited due to the instability of this phase. Here, we report a simple ambient temperature modification method using sonication to dope the single layer 1T-SMoS2 with various TM precursors. It is found that 1T-SMoS2 is more active than corresponding 2H-SMoS2 and the inclusion of 3 wt % Pt or Pd can also further enhance the HER activity. STEM-EELS and XAS show that the active single TM atom doping on this surface accounts for the high activity. Kinetic and DFT analyses also illustrate that the metallic nature of 1T-SMoS2 greatly facilitates the proton reduction step from water, rendering it non-rate-limiting in contrast to that of 2H-SMoS2. The inclusion of the TM single doper such as Pd, despite at low loading, can offer the dramatic acceleration of the rate limiting recombination of H to H2. As a result, a bifunctional catalysis for HER over this tailored composite structure is demonstrated that outperforms most reported catalysts in this area.
first_indexed 2024-03-06T23:54:24Z
format Journal article
id oxford-uuid:73b2f014-3f09-42ee-8108-418bf34bacda
institution University of Oxford
language English
last_indexed 2024-03-06T23:54:24Z
publishDate 2019
publisher American Chemical Society
record_format dspace
spelling oxford-uuid:73b2f014-3f09-42ee-8108-418bf34bacda2022-03-26T19:58:13ZEngineering monolayer 1T-MoS2 into a bifunctional electrocatalyst via sonochemical doping of isolated transition metal atomsJournal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:73b2f014-3f09-42ee-8108-418bf34bacdaEnglishSymplectic ElementsAmerican Chemical Society2019Lau, THMWu, SKato, RWu, T-SKulhavy, JMo, JZheng, JFoord, JSSoo, Y-LSuenaga, KDarby, MTTsang, SCEThere has been an intense research effort to develop 2-H MoS2 based catalysts to reduce or eliminate the use of Pt/C at higher metal loading for the hydrogen evolution reaction (HER) in catalytic hydrolysis of water, which enables the capture of renewable energy sources as fuel and chemical. However, the study of its uncommon polymorph, 1T-MoS2, and particularly the doping effect with transition metal (TM) is rather limited due to the instability of this phase. Here, we report a simple ambient temperature modification method using sonication to dope the single layer 1T-SMoS2 with various TM precursors. It is found that 1T-SMoS2 is more active than corresponding 2H-SMoS2 and the inclusion of 3 wt % Pt or Pd can also further enhance the HER activity. STEM-EELS and XAS show that the active single TM atom doping on this surface accounts for the high activity. Kinetic and DFT analyses also illustrate that the metallic nature of 1T-SMoS2 greatly facilitates the proton reduction step from water, rendering it non-rate-limiting in contrast to that of 2H-SMoS2. The inclusion of the TM single doper such as Pd, despite at low loading, can offer the dramatic acceleration of the rate limiting recombination of H to H2. As a result, a bifunctional catalysis for HER over this tailored composite structure is demonstrated that outperforms most reported catalysts in this area.
spellingShingle Lau, THM
Wu, S
Kato, R
Wu, T-S
Kulhavy, J
Mo, J
Zheng, J
Foord, JS
Soo, Y-L
Suenaga, K
Darby, MT
Tsang, SCE
Engineering monolayer 1T-MoS2 into a bifunctional electrocatalyst via sonochemical doping of isolated transition metal atoms
title Engineering monolayer 1T-MoS2 into a bifunctional electrocatalyst via sonochemical doping of isolated transition metal atoms
title_full Engineering monolayer 1T-MoS2 into a bifunctional electrocatalyst via sonochemical doping of isolated transition metal atoms
title_fullStr Engineering monolayer 1T-MoS2 into a bifunctional electrocatalyst via sonochemical doping of isolated transition metal atoms
title_full_unstemmed Engineering monolayer 1T-MoS2 into a bifunctional electrocatalyst via sonochemical doping of isolated transition metal atoms
title_short Engineering monolayer 1T-MoS2 into a bifunctional electrocatalyst via sonochemical doping of isolated transition metal atoms
title_sort engineering monolayer 1t mos2 into a bifunctional electrocatalyst via sonochemical doping of isolated transition metal atoms
work_keys_str_mv AT lauthm engineeringmonolayer1tmos2intoabifunctionalelectrocatalystviasonochemicaldopingofisolatedtransitionmetalatoms
AT wus engineeringmonolayer1tmos2intoabifunctionalelectrocatalystviasonochemicaldopingofisolatedtransitionmetalatoms
AT kator engineeringmonolayer1tmos2intoabifunctionalelectrocatalystviasonochemicaldopingofisolatedtransitionmetalatoms
AT wuts engineeringmonolayer1tmos2intoabifunctionalelectrocatalystviasonochemicaldopingofisolatedtransitionmetalatoms
AT kulhavyj engineeringmonolayer1tmos2intoabifunctionalelectrocatalystviasonochemicaldopingofisolatedtransitionmetalatoms
AT moj engineeringmonolayer1tmos2intoabifunctionalelectrocatalystviasonochemicaldopingofisolatedtransitionmetalatoms
AT zhengj engineeringmonolayer1tmos2intoabifunctionalelectrocatalystviasonochemicaldopingofisolatedtransitionmetalatoms
AT foordjs engineeringmonolayer1tmos2intoabifunctionalelectrocatalystviasonochemicaldopingofisolatedtransitionmetalatoms
AT sooyl engineeringmonolayer1tmos2intoabifunctionalelectrocatalystviasonochemicaldopingofisolatedtransitionmetalatoms
AT suenagak engineeringmonolayer1tmos2intoabifunctionalelectrocatalystviasonochemicaldopingofisolatedtransitionmetalatoms
AT darbymt engineeringmonolayer1tmos2intoabifunctionalelectrocatalystviasonochemicaldopingofisolatedtransitionmetalatoms
AT tsangsce engineeringmonolayer1tmos2intoabifunctionalelectrocatalystviasonochemicaldopingofisolatedtransitionmetalatoms