Edge-site nano-engineering of WS2 by low temperature plasma-enhanced atomic layer deposition for electrocatalytic hydrogen evolution

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Uittreksel

Edge-enriched transition metal dichalcogenides (TMDs) like WS2 are promising electrocatalysts for sustainable production of H2 through the electrochemical hydrogen evolution reaction (HER). The reliable and controlled growth of such edge-enriched electrocatalysts at low temperatures has, however, remained elusive. In this work, we demonstrate how plasma-enhanced atomic layer deposition (PEALD) can be used as a new approach to nano-engineer and enhance the HER performance of WS2 by maximizing the density of reactive edge sites at a low temperature of 300 °C. By altering the plasma gas composition from H2S to H2+H2S during PEALD, we could precisely control the morphology and composition, and consequently, the edge-site density as well as chemistry in our WS2 films. The precise control over edge-site density was verified by evaluating the number of exposed edge-sites using electrochemical copper underpotential depositions (Cu-UPD). Subsequently, we demonstrate the HER performance of the edge-enriched WS2 electrocatalyst, and a clear correlation between plasma conditions, edge-site density and the HER performance is obtained. Additionally, using density functional theory (DFT) calculations we provide insights and explain how the addition of H2 to the H2S plasma impacts the PEALD growth behaviour, and consequently, the material properties, when compared to H2S plasma only.
TaalEngels
Pagina's5104-5115
TijdschriftChemistry of Materials
Volume31
Nummer van het tijdschrift14
DOI's
StatusGepubliceerd - 25 jun 2019

Vingerafdruk

Atomic layer deposition
Hydrogen
Plasmas
Electrocatalysts
Temperature
Plasma Gases
Chemical analysis
Transition metals
Density functional theory
Copper
Materials properties
Engineers
Gases

Citeer dit

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title = "Edge-site nano-engineering of WS2 by low temperature plasma-enhanced atomic layer deposition for electrocatalytic hydrogen evolution",
abstract = "Edge-enriched transition metal dichalcogenides (TMDs) like WS2 are promising electrocatalysts for sustainable production of H2 through the electrochemical hydrogen evolution reaction (HER). The reliable and controlled growth of such edge-enriched electrocatalysts at low temperatures has, however, remained elusive. In this work, we demonstrate how plasma-enhanced atomic layer deposition (PEALD) can be used as a new approach to nano-engineer and enhance the HER performance of WS2 by maximizing the density of reactive edge sites at a low temperature of 300 °C. By altering the plasma gas composition from H2S to H2+H2S during PEALD, we could precisely control the morphology and composition, and consequently, the edge-site density as well as chemistry in our WS2 films. The precise control over edge-site density was verified by evaluating the number of exposed edge-sites using electrochemical copper underpotential depositions (Cu-UPD). Subsequently, we demonstrate the HER performance of the edge-enriched WS2 electrocatalyst, and a clear correlation between plasma conditions, edge-site density and the HER performance is obtained. Additionally, using density functional theory (DFT) calculations we provide insights and explain how the addition of H2 to the H2S plasma impacts the PEALD growth behaviour, and consequently, the material properties, when compared to H2S plasma only.",
author = "Shashank Balasubramanyam and Mahdi Shirazi and Matthew Bloodgood and Longfei Wu and Marcel Verheijen and Vincent Vandalon and Erwin Kessels and Hofmann, {Jan Philipp} and Bol, {Ageeth A.}",
year = "2019",
month = "6",
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doi = "10.1021/acs.chemmater.9b01008",
language = "English",
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journal = "Chemistry of Materials",
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publisher = "American Chemical Society",
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T1 - Edge-site nano-engineering of WS2 by low temperature plasma-enhanced atomic layer deposition for electrocatalytic hydrogen evolution

AU - Balasubramanyam,Shashank

AU - Shirazi,Mahdi

AU - Bloodgood,Matthew

AU - Wu,Longfei

AU - Verheijen,Marcel

AU - Vandalon,Vincent

AU - Kessels,Erwin

AU - Hofmann,Jan Philipp

AU - Bol,Ageeth A.

PY - 2019/6/25

Y1 - 2019/6/25

N2 - Edge-enriched transition metal dichalcogenides (TMDs) like WS2 are promising electrocatalysts for sustainable production of H2 through the electrochemical hydrogen evolution reaction (HER). The reliable and controlled growth of such edge-enriched electrocatalysts at low temperatures has, however, remained elusive. In this work, we demonstrate how plasma-enhanced atomic layer deposition (PEALD) can be used as a new approach to nano-engineer and enhance the HER performance of WS2 by maximizing the density of reactive edge sites at a low temperature of 300 °C. By altering the plasma gas composition from H2S to H2+H2S during PEALD, we could precisely control the morphology and composition, and consequently, the edge-site density as well as chemistry in our WS2 films. The precise control over edge-site density was verified by evaluating the number of exposed edge-sites using electrochemical copper underpotential depositions (Cu-UPD). Subsequently, we demonstrate the HER performance of the edge-enriched WS2 electrocatalyst, and a clear correlation between plasma conditions, edge-site density and the HER performance is obtained. Additionally, using density functional theory (DFT) calculations we provide insights and explain how the addition of H2 to the H2S plasma impacts the PEALD growth behaviour, and consequently, the material properties, when compared to H2S plasma only.

AB - Edge-enriched transition metal dichalcogenides (TMDs) like WS2 are promising electrocatalysts for sustainable production of H2 through the electrochemical hydrogen evolution reaction (HER). The reliable and controlled growth of such edge-enriched electrocatalysts at low temperatures has, however, remained elusive. In this work, we demonstrate how plasma-enhanced atomic layer deposition (PEALD) can be used as a new approach to nano-engineer and enhance the HER performance of WS2 by maximizing the density of reactive edge sites at a low temperature of 300 °C. By altering the plasma gas composition from H2S to H2+H2S during PEALD, we could precisely control the morphology and composition, and consequently, the edge-site density as well as chemistry in our WS2 films. The precise control over edge-site density was verified by evaluating the number of exposed edge-sites using electrochemical copper underpotential depositions (Cu-UPD). Subsequently, we demonstrate the HER performance of the edge-enriched WS2 electrocatalyst, and a clear correlation between plasma conditions, edge-site density and the HER performance is obtained. Additionally, using density functional theory (DFT) calculations we provide insights and explain how the addition of H2 to the H2S plasma impacts the PEALD growth behaviour, and consequently, the material properties, when compared to H2S plasma only.

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