Uittreksel
Edge-enriched transition metal dichalcogenides, such as WS 2, are promising electrocatalysts for sustainable production of H 2 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 nanoengineer and enhance the HER performance of WS 2 by maximizing the density of reactive edge sites at a low temperature of 300 °C. By altering the plasma gas composition from H 2S to H 2 + H 2S during PEALD, we could precisely control the morphology and composition and, consequently, the edge-site density as well as chemistry in our WS 2 films. The precise control over edge-site density was verified by evaluating the number of exposed edge sites using electrochemical copper underpotential depositions. Subsequently, we demonstrate the HER performance of the edge-enriched WS 2 electrocatalyst, and a clear correlation among plasma conditions, edge-site density, and the HER performance is obtained. Additionally, using density functional theory calculations we provide insights and explain how the addition of H 2 to the H 2S plasma impacts the PEALD growth behavior and, consequently, the material properties, when compared to only H 2S plasma.
| Originele taal-2 | Engels |
|---|---|
| Pagina's (van-tot) | 5104-5115 |
| Aantal pagina's | 12 |
| Tijdschrift | Chemistry of Materials |
| Volume | 31 |
| Nummer van het tijdschrift | 14 |
| DOI's | |
| Status | Gepubliceerd - 25 jun 2019 |
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Edge-site nano-engineering of WS2 by low temperature plasma-enhanced atomic layer deposition for electrocatalytic hydrogen evolution. / Balasubramanyam, Shashank; Shirazi, Mahdi; Bloodgood, Matthew; Wu, Longfei; Verheijen, Marcel; Vandalon, Vincent; Kessels, Erwin; Hofmann, Jan Philipp; Bol, Ageeth A. (Corresponding author).
In: Chemistry of Materials, Vol. 31, Nr. 14, 25.06.2019, blz. 5104-5115.Onderzoeksoutput: Bijdrage aan tijdschrift › Tijdschriftartikel › Academic › peer review
TY - JOUR
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, such as WS 2, are promising electrocatalysts for sustainable production of H 2 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 nanoengineer and enhance the HER performance of WS 2 by maximizing the density of reactive edge sites at a low temperature of 300 °C. By altering the plasma gas composition from H 2S to H 2 + H 2S during PEALD, we could precisely control the morphology and composition and, consequently, the edge-site density as well as chemistry in our WS 2 films. The precise control over edge-site density was verified by evaluating the number of exposed edge sites using electrochemical copper underpotential depositions. Subsequently, we demonstrate the HER performance of the edge-enriched WS 2 electrocatalyst, and a clear correlation among plasma conditions, edge-site density, and the HER performance is obtained. Additionally, using density functional theory calculations we provide insights and explain how the addition of H 2 to the H 2S plasma impacts the PEALD growth behavior and, consequently, the material properties, when compared to only H 2S plasma.
AB - Edge-enriched transition metal dichalcogenides, such as WS 2, are promising electrocatalysts for sustainable production of H 2 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 nanoengineer and enhance the HER performance of WS 2 by maximizing the density of reactive edge sites at a low temperature of 300 °C. By altering the plasma gas composition from H 2S to H 2 + H 2S during PEALD, we could precisely control the morphology and composition and, consequently, the edge-site density as well as chemistry in our WS 2 films. The precise control over edge-site density was verified by evaluating the number of exposed edge sites using electrochemical copper underpotential depositions. Subsequently, we demonstrate the HER performance of the edge-enriched WS 2 electrocatalyst, and a clear correlation among plasma conditions, edge-site density, and the HER performance is obtained. Additionally, using density functional theory calculations we provide insights and explain how the addition of H 2 to the H 2S plasma impacts the PEALD growth behavior and, consequently, the material properties, when compared to only H 2S plasma.
UR - http://www.scopus.com/inward/record.url?scp=85070541798&partnerID=8YFLogxK
U2 - 10.1021/acs.chemmater.9b01008
DO - 10.1021/acs.chemmater.9b01008
M3 - Article
C2 - 31371869
VL - 31
SP - 5104
EP - 5115
JO - Chemistry of Materials
JF - Chemistry of Materials
SN - 0897-4756
IS - 14
ER -