Rapid flame doping of Co to WS2 for efficient hydrogen evolution

Xinjian Shi, Meredith Fields, Joonsuk Park, Joshua M. McEnaney, Hongping Yan, Yirui Zhang, Charlie Tsai, Thomas F. Jaramillo, Robert Sinclair, Jens K. Nørskov*, Xiaolin Zheng

*Corresponding author for this work

Research output: Contribution to journalJournal articleResearchpeer-review

Abstract

Transition metal sulfides have been widely studied as electrocatalysts for the hydrogen evolution reaction (HER). Though elemental doping is an effective way to enhance sulfide activity for the HER, most studies have only focused on the effect of doping sulfide edge sites. Few studies have investigated the effect of doping the basal plane or the effect of doping concentration on basal plane activity. Probing the dopant concentration dependence of HER activity is challenging due to experimental difficulties in controlling dopant incorporation. Here, we overcome this challenge by first synthesizing doped transition metal oxides and then sulfurizing the oxides to sulfides, yielding core/shell Co-doped WS2/W18O49 nanotubes with a tunable amount of Co. Our combined density functional theory (DFT) calculations and experiments demonstrate that the HER activity of basal plane WS2 changes non-monotonically with the concentration of Co due to local changes in the binding energy of H and the formation energy of S-vacancies. At an optimal Co doping concentration, the overpotential to reach -10 mA cm-2 is reduced by 210 mV, and the Tafel slope is reduced from 122 to 49 mV per decade (mV dec-1) compared to undoped WS2 nanotubes.

Original languageEnglish
JournalEnergy and Environmental Science
Volume11
Issue number8
Pages (from-to)2270-2277
ISSN1754-5692
DOIs
Publication statusPublished - 2018
Externally publishedYes

Cite this

Shi, X., Fields, M., Park, J., McEnaney, J. M., Yan, H., Zhang, Y., ... Zheng, X. (2018). Rapid flame doping of Co to WS2 for efficient hydrogen evolution. Energy and Environmental Science, 11(8), 2270-2277. https://doi.org/10.1039/c8ee01111g
Shi, Xinjian ; Fields, Meredith ; Park, Joonsuk ; McEnaney, Joshua M. ; Yan, Hongping ; Zhang, Yirui ; Tsai, Charlie ; Jaramillo, Thomas F. ; Sinclair, Robert ; Nørskov, Jens K. ; Zheng, Xiaolin. / Rapid flame doping of Co to WS2 for efficient hydrogen evolution. In: Energy and Environmental Science. 2018 ; Vol. 11, No. 8. pp. 2270-2277.
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title = "Rapid flame doping of Co to WS2 for efficient hydrogen evolution",
abstract = "Transition metal sulfides have been widely studied as electrocatalysts for the hydrogen evolution reaction (HER). Though elemental doping is an effective way to enhance sulfide activity for the HER, most studies have only focused on the effect of doping sulfide edge sites. Few studies have investigated the effect of doping the basal plane or the effect of doping concentration on basal plane activity. Probing the dopant concentration dependence of HER activity is challenging due to experimental difficulties in controlling dopant incorporation. Here, we overcome this challenge by first synthesizing doped transition metal oxides and then sulfurizing the oxides to sulfides, yielding core/shell Co-doped WS2/W18O49 nanotubes with a tunable amount of Co. Our combined density functional theory (DFT) calculations and experiments demonstrate that the HER activity of basal plane WS2 changes non-monotonically with the concentration of Co due to local changes in the binding energy of H and the formation energy of S-vacancies. At an optimal Co doping concentration, the overpotential to reach -10 mA cm-2 is reduced by 210 mV, and the Tafel slope is reduced from 122 to 49 mV per decade (mV dec-1) compared to undoped WS2 nanotubes.",
author = "Xinjian Shi and Meredith Fields and Joonsuk Park and McEnaney, {Joshua M.} and Hongping Yan and Yirui Zhang and Charlie Tsai and Jaramillo, {Thomas F.} and Robert Sinclair and N{\o}rskov, {Jens K.} and Xiaolin Zheng",
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language = "English",
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Shi, X, Fields, M, Park, J, McEnaney, JM, Yan, H, Zhang, Y, Tsai, C, Jaramillo, TF, Sinclair, R, Nørskov, JK & Zheng, X 2018, 'Rapid flame doping of Co to WS2 for efficient hydrogen evolution', Energy and Environmental Science, vol. 11, no. 8, pp. 2270-2277. https://doi.org/10.1039/c8ee01111g

Rapid flame doping of Co to WS2 for efficient hydrogen evolution. / Shi, Xinjian; Fields, Meredith; Park, Joonsuk; McEnaney, Joshua M.; Yan, Hongping; Zhang, Yirui; Tsai, Charlie; Jaramillo, Thomas F.; Sinclair, Robert; Nørskov, Jens K.; Zheng, Xiaolin.

In: Energy and Environmental Science, Vol. 11, No. 8, 2018, p. 2270-2277.

Research output: Contribution to journalJournal articleResearchpeer-review

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T1 - Rapid flame doping of Co to WS2 for efficient hydrogen evolution

AU - Shi, Xinjian

AU - Fields, Meredith

AU - Park, Joonsuk

AU - McEnaney, Joshua M.

AU - Yan, Hongping

AU - Zhang, Yirui

AU - Tsai, Charlie

AU - Jaramillo, Thomas F.

AU - Sinclair, Robert

AU - Nørskov, Jens K.

AU - Zheng, Xiaolin

PY - 2018

Y1 - 2018

N2 - Transition metal sulfides have been widely studied as electrocatalysts for the hydrogen evolution reaction (HER). Though elemental doping is an effective way to enhance sulfide activity for the HER, most studies have only focused on the effect of doping sulfide edge sites. Few studies have investigated the effect of doping the basal plane or the effect of doping concentration on basal plane activity. Probing the dopant concentration dependence of HER activity is challenging due to experimental difficulties in controlling dopant incorporation. Here, we overcome this challenge by first synthesizing doped transition metal oxides and then sulfurizing the oxides to sulfides, yielding core/shell Co-doped WS2/W18O49 nanotubes with a tunable amount of Co. Our combined density functional theory (DFT) calculations and experiments demonstrate that the HER activity of basal plane WS2 changes non-monotonically with the concentration of Co due to local changes in the binding energy of H and the formation energy of S-vacancies. At an optimal Co doping concentration, the overpotential to reach -10 mA cm-2 is reduced by 210 mV, and the Tafel slope is reduced from 122 to 49 mV per decade (mV dec-1) compared to undoped WS2 nanotubes.

AB - Transition metal sulfides have been widely studied as electrocatalysts for the hydrogen evolution reaction (HER). Though elemental doping is an effective way to enhance sulfide activity for the HER, most studies have only focused on the effect of doping sulfide edge sites. Few studies have investigated the effect of doping the basal plane or the effect of doping concentration on basal plane activity. Probing the dopant concentration dependence of HER activity is challenging due to experimental difficulties in controlling dopant incorporation. Here, we overcome this challenge by first synthesizing doped transition metal oxides and then sulfurizing the oxides to sulfides, yielding core/shell Co-doped WS2/W18O49 nanotubes with a tunable amount of Co. Our combined density functional theory (DFT) calculations and experiments demonstrate that the HER activity of basal plane WS2 changes non-monotonically with the concentration of Co due to local changes in the binding energy of H and the formation energy of S-vacancies. At an optimal Co doping concentration, the overpotential to reach -10 mA cm-2 is reduced by 210 mV, and the Tafel slope is reduced from 122 to 49 mV per decade (mV dec-1) compared to undoped WS2 nanotubes.

U2 - 10.1039/c8ee01111g

DO - 10.1039/c8ee01111g

M3 - Journal article

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SP - 2270

EP - 2277

JO - Energy & Environmental Science

JF - Energy & Environmental Science

SN - 1754-5692

IS - 8

ER -