Abstract
Low-dimensional materials have been examined as electrocatalysts for the hydrogen evolution reaction (HER). Among them, two-dimensional transition metal dichalcogenides (2D-TMDs) such as MoS2 have been identified as potential candidates. However, the performance of TMDs toward HER in both acidic and basic media remains inferior to that of noble metals such as Pt and its alloys. This calls for investigating the influence of controlled defect engineering of 2D TMDs on their performance toward hydrogen production. Here, we explored the HER activity from defective multilayered MoS2 over a large range of surface S vacancy concentrations up to 90%. Amorphous MoS2 and 2H MoS2 with ultrarich S vacancies demonstrated the highest HER performance in acid and basic electrolytes, respectively. We also report that the HER performance from multilayered MoS2 can be divided into two domains corresponding to "point defects" at low concentrations of surface S vacancies (Stage 1) and large regions of undercoordinated Mo atoms for high concentrations of surface S vacancies (Stage 2). The highest performance is obtained for Stage 2 in the presence of undercoordinated Mo atoms with a TOF of ∼2 s-1 at an overpotential of 160 mV in 0.1 M KOH which compares favorably to the best results in the literature. Overall, our work provides deeper insight on the HER mechanism from defected MoS2 and provides guidance for the development of defect-engineered TMD-based electrocatalysts.
| Original language | English |
|---|---|
| Journal | ACS nano |
| DOIs | |
| Publication status | Published - Jan 1 2019 |
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Keywords
- H-annealing
- hydrogen evolution reaction
- MoS
- sulfur vacancies
- undercoordinated Mo
ASJC Scopus subject areas
- Materials Science(all)
- Engineering(all)
- Physics and Astronomy(all)
Cite this
Role of Sulfur Vacancies and Undercoordinated Mo Regions in MoS2 Nanosheets toward the Evolution of Hydrogen. / Li, Lei; Qin, Zhaodan; Ries, Lucie; Hong, Song; Michel, Thierry; Yang, Jieun; Salameh, Chrystelle; Bechelany, Mikhael; Miele, Philippe; Kaplan, Daniel; Chhowalla, Manish; Voiry, Damien.
In: ACS nano, 01.01.2019.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Role of Sulfur Vacancies and Undercoordinated Mo Regions in MoS2 Nanosheets toward the Evolution of Hydrogen
AU - Li, Lei
AU - Qin, Zhaodan
AU - Ries, Lucie
AU - Hong, Song
AU - Michel, Thierry
AU - Yang, Jieun
AU - Salameh, Chrystelle
AU - Bechelany, Mikhael
AU - Miele, Philippe
AU - Kaplan, Daniel
AU - Chhowalla, Manish
AU - Voiry, Damien
PY - 2019/1/1
Y1 - 2019/1/1
N2 - Low-dimensional materials have been examined as electrocatalysts for the hydrogen evolution reaction (HER). Among them, two-dimensional transition metal dichalcogenides (2D-TMDs) such as MoS2 have been identified as potential candidates. However, the performance of TMDs toward HER in both acidic and basic media remains inferior to that of noble metals such as Pt and its alloys. This calls for investigating the influence of controlled defect engineering of 2D TMDs on their performance toward hydrogen production. Here, we explored the HER activity from defective multilayered MoS2 over a large range of surface S vacancy concentrations up to 90%. Amorphous MoS2 and 2H MoS2 with ultrarich S vacancies demonstrated the highest HER performance in acid and basic electrolytes, respectively. We also report that the HER performance from multilayered MoS2 can be divided into two domains corresponding to "point defects" at low concentrations of surface S vacancies (Stage 1) and large regions of undercoordinated Mo atoms for high concentrations of surface S vacancies (Stage 2). The highest performance is obtained for Stage 2 in the presence of undercoordinated Mo atoms with a TOF of ∼2 s-1 at an overpotential of 160 mV in 0.1 M KOH which compares favorably to the best results in the literature. Overall, our work provides deeper insight on the HER mechanism from defected MoS2 and provides guidance for the development of defect-engineered TMD-based electrocatalysts.
AB - Low-dimensional materials have been examined as electrocatalysts for the hydrogen evolution reaction (HER). Among them, two-dimensional transition metal dichalcogenides (2D-TMDs) such as MoS2 have been identified as potential candidates. However, the performance of TMDs toward HER in both acidic and basic media remains inferior to that of noble metals such as Pt and its alloys. This calls for investigating the influence of controlled defect engineering of 2D TMDs on their performance toward hydrogen production. Here, we explored the HER activity from defective multilayered MoS2 over a large range of surface S vacancy concentrations up to 90%. Amorphous MoS2 and 2H MoS2 with ultrarich S vacancies demonstrated the highest HER performance in acid and basic electrolytes, respectively. We also report that the HER performance from multilayered MoS2 can be divided into two domains corresponding to "point defects" at low concentrations of surface S vacancies (Stage 1) and large regions of undercoordinated Mo atoms for high concentrations of surface S vacancies (Stage 2). The highest performance is obtained for Stage 2 in the presence of undercoordinated Mo atoms with a TOF of ∼2 s-1 at an overpotential of 160 mV in 0.1 M KOH which compares favorably to the best results in the literature. Overall, our work provides deeper insight on the HER mechanism from defected MoS2 and provides guidance for the development of defect-engineered TMD-based electrocatalysts.
KW - H-annealing
KW - hydrogen evolution reaction
KW - MoS
KW - sulfur vacancies
KW - undercoordinated Mo
UR - http://www.scopus.com/inward/record.url?scp=85067400956&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85067400956&partnerID=8YFLogxK
U2 - 10.1021/acsnano.9b01583
DO - 10.1021/acsnano.9b01583
M3 - Article
C2 - 31136708
AN - SCOPUS:85067400956
JO - ACS Nano
JF - ACS Nano
SN - 1936-0851
ER -