Aligned Heterointerface-Induced 1T-MoS 2 Monolayer with Near-Ideal Gibbs Free for Stable Hydrogen Evolution Reaction

Kan Zhang, Bingjun Jin, Yujie Gao, Shengli Zhang, Hyunjung Shin, Haibo Zeng, Jong Hyeok Park

Research output: Contribution to journalArticle

5 Citations (Scopus)

Abstract

1T-phase molybdenum disulfide (1T-MoS 2 ) exhibits superior hydrogen evolution reaction (HER) over 2H-phase MoS 2 (2H-MoS 2 ). However, its thermodynamic instability is the main drawback impeding its practical application. In this work, a stable 1T-MoS 2 monolayer formed at edge-aligned 2H-MoS 2 and a reduced graphene oxide heterointerface (EA-2H/1T/RGO) using a precursor-in-solvent synthesis strategy are reported. Theoretical prediction indicates that the edge-aligned layer stacking can induce heterointerfacial charge transfer, which results in a phase transition of the interfacial monolayer from 2H to 1T that realizes thermodynamic stability based on the adhesion energy between MoS 2 and graphene. As an electrocatalyst for HER, EA-2H/1T/RGO displays an onset potential of −103 mV versus RHE, a Tafel slope of 46 mV dec −1 and 10 h stability in acidic electrolyte. The unexpected activity of EA-2H/1T/RGO beyond 1T-MoS 2 is due to an inherent defect caused by the gliding of S atoms during the phase transition from 2H to 1T, leading the Gibbs free energy of hydrogen adsorption (ΔG H* ) to decrease from 0.13 to 0.07 eV, which is closest to the ideal value (0.06 eV) of 2H-MoS 2 . The presented work provides fundamental insights into the impressive electrochemical properties of HER and opens new avenues for phase transitions at 2D/2D hybrid interfaces.

Original languageEnglish
Article number1804903
JournalSmall
Volume15
Issue number8
DOIs
Publication statusPublished - 2019 Feb 22

Fingerprint

Hydrogen
Monolayers
Phase Transition
Graphite
Phase transitions
Thermodynamics
Graphene
Electrocatalysts
Gibbs free energy
Electrochemical properties
Oxides
Electrolytes
Adsorption
Charge transfer
Thermodynamic stability
Adhesion
Molybdenum
Atoms
Defects

All Science Journal Classification (ASJC) codes

  • Biotechnology
  • Biomaterials
  • Chemistry(all)
  • Materials Science(all)

Cite this

Zhang, Kan ; Jin, Bingjun ; Gao, Yujie ; Zhang, Shengli ; Shin, Hyunjung ; Zeng, Haibo ; Park, Jong Hyeok. / Aligned Heterointerface-Induced 1T-MoS 2 Monolayer with Near-Ideal Gibbs Free for Stable Hydrogen Evolution Reaction In: Small. 2019 ; Vol. 15, No. 8.
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abstract = "1T-phase molybdenum disulfide (1T-MoS 2 ) exhibits superior hydrogen evolution reaction (HER) over 2H-phase MoS 2 (2H-MoS 2 ). However, its thermodynamic instability is the main drawback impeding its practical application. In this work, a stable 1T-MoS 2 monolayer formed at edge-aligned 2H-MoS 2 and a reduced graphene oxide heterointerface (EA-2H/1T/RGO) using a precursor-in-solvent synthesis strategy are reported. Theoretical prediction indicates that the edge-aligned layer stacking can induce heterointerfacial charge transfer, which results in a phase transition of the interfacial monolayer from 2H to 1T that realizes thermodynamic stability based on the adhesion energy between MoS 2 and graphene. As an electrocatalyst for HER, EA-2H/1T/RGO displays an onset potential of −103 mV versus RHE, a Tafel slope of 46 mV dec −1 and 10 h stability in acidic electrolyte. The unexpected activity of EA-2H/1T/RGO beyond 1T-MoS 2 is due to an inherent defect caused by the gliding of S atoms during the phase transition from 2H to 1T, leading the Gibbs free energy of hydrogen adsorption (ΔG H* ) to decrease from 0.13 to 0.07 eV, which is closest to the ideal value (0.06 eV) of 2H-MoS 2 . The presented work provides fundamental insights into the impressive electrochemical properties of HER and opens new avenues for phase transitions at 2D/2D hybrid interfaces.",
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Aligned Heterointerface-Induced 1T-MoS 2 Monolayer with Near-Ideal Gibbs Free for Stable Hydrogen Evolution Reaction . / Zhang, Kan; Jin, Bingjun; Gao, Yujie; Zhang, Shengli; Shin, Hyunjung; Zeng, Haibo; Park, Jong Hyeok.

In: Small, Vol. 15, No. 8, 1804903, 22.02.2019.

Research output: Contribution to journalArticle

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T1 - Aligned Heterointerface-Induced 1T-MoS 2 Monolayer with Near-Ideal Gibbs Free for Stable Hydrogen Evolution Reaction

AU - Zhang, Kan

AU - Jin, Bingjun

AU - Gao, Yujie

AU - Zhang, Shengli

AU - Shin, Hyunjung

AU - Zeng, Haibo

AU - Park, Jong Hyeok

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N2 - 1T-phase molybdenum disulfide (1T-MoS 2 ) exhibits superior hydrogen evolution reaction (HER) over 2H-phase MoS 2 (2H-MoS 2 ). However, its thermodynamic instability is the main drawback impeding its practical application. In this work, a stable 1T-MoS 2 monolayer formed at edge-aligned 2H-MoS 2 and a reduced graphene oxide heterointerface (EA-2H/1T/RGO) using a precursor-in-solvent synthesis strategy are reported. Theoretical prediction indicates that the edge-aligned layer stacking can induce heterointerfacial charge transfer, which results in a phase transition of the interfacial monolayer from 2H to 1T that realizes thermodynamic stability based on the adhesion energy between MoS 2 and graphene. As an electrocatalyst for HER, EA-2H/1T/RGO displays an onset potential of −103 mV versus RHE, a Tafel slope of 46 mV dec −1 and 10 h stability in acidic electrolyte. The unexpected activity of EA-2H/1T/RGO beyond 1T-MoS 2 is due to an inherent defect caused by the gliding of S atoms during the phase transition from 2H to 1T, leading the Gibbs free energy of hydrogen adsorption (ΔG H* ) to decrease from 0.13 to 0.07 eV, which is closest to the ideal value (0.06 eV) of 2H-MoS 2 . The presented work provides fundamental insights into the impressive electrochemical properties of HER and opens new avenues for phase transitions at 2D/2D hybrid interfaces.

AB - 1T-phase molybdenum disulfide (1T-MoS 2 ) exhibits superior hydrogen evolution reaction (HER) over 2H-phase MoS 2 (2H-MoS 2 ). However, its thermodynamic instability is the main drawback impeding its practical application. In this work, a stable 1T-MoS 2 monolayer formed at edge-aligned 2H-MoS 2 and a reduced graphene oxide heterointerface (EA-2H/1T/RGO) using a precursor-in-solvent synthesis strategy are reported. Theoretical prediction indicates that the edge-aligned layer stacking can induce heterointerfacial charge transfer, which results in a phase transition of the interfacial monolayer from 2H to 1T that realizes thermodynamic stability based on the adhesion energy between MoS 2 and graphene. As an electrocatalyst for HER, EA-2H/1T/RGO displays an onset potential of −103 mV versus RHE, a Tafel slope of 46 mV dec −1 and 10 h stability in acidic electrolyte. The unexpected activity of EA-2H/1T/RGO beyond 1T-MoS 2 is due to an inherent defect caused by the gliding of S atoms during the phase transition from 2H to 1T, leading the Gibbs free energy of hydrogen adsorption (ΔG H* ) to decrease from 0.13 to 0.07 eV, which is closest to the ideal value (0.06 eV) of 2H-MoS 2 . The presented work provides fundamental insights into the impressive electrochemical properties of HER and opens new avenues for phase transitions at 2D/2D hybrid interfaces.

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