Wide Range pH-Tolerable Silicon@Pyrite Cobalt Dichalcogenide Microwire Array Photoelectrodes for Solar Hydrogen Evolution

Chih Jung Chen, Kai Chih Yang, Mrinmoyee Basu, Tzu Hsiang Lu, Ying Rui Lu, Chung Li Dong, Shu Fen Hu, Ru Shi Liu

Research output: Contribution to journalArticle

13 Citations (Scopus)

Abstract

This study employed silicon@cobalt dichalcogenide microwires (MWs) as wide range pH-tolerable photocathode material for solar water splitting. Silicon microwire arrays were fabricated through lithography and dry etching technologies. Si@Co(OH)2 MWs were utilized as precursors to synthesize Si@CoX2 (X = S or Se) photocathodes. Si@CoS2 and Si@CoSe2 MWs were subsequently prepared by thermal sulfidation and hydrothermal selenization reaction of Si@Co(OH)2, respectively. The CoX2 outer shell served as cocatalyst to accelerate the kinetics of photogenerated electrons from the underlying Si MWs and reduce the recombination. Moreover, the CoX2 layer completely deposited on the Si surface functioned as a passivation layer by decreasing the oxide formation on Si MWs during solar hydrogen evolution. Si@CoS2 photocathode showed a photocurrent density of -3.22 mA cm-2 at 0 V (vs RHE) in 0.5 M sulfuric acid electrolyte, and Si@CoSe2 MWs revealed moderate photocurrent density of -2.55 mA cm-2. However, Si@CoSe2 presented high charge transfer efficiency in neutral and alkaline electrolytes. Continuous chronoamperometry in acid, neutral, and alkaline solutions was conducted at 0 V (vs RHE) to evaluate the photoelectrochemical durability of Si@CoX2 MWs. Si@CoS2 electrode showed no photoresponse after the chronoamperometry test because it was etched through the electrolyte. By contrast, the photocurrent density of Si@CoSe2 MWs gradually increased to -5 mA cm-2 after chronoamperometry characterization owing to the amorphous structure generation.

Original languageEnglish
Pages (from-to)5400-5407
Number of pages8
JournalACS Applied Materials and Interfaces
Volume8
Issue number8
DOIs
Publication statusPublished - 2016 Mar 2

Fingerprint

Chronoamperometry
Photocathodes
Pyrites
Silicon
Cobalt
Photocurrents
Electrolytes
Hydrogen
Dry etching
Sulfuric acid
Passivation
Oxides
Lithography
Charge transfer
Durability
Electrodes
Kinetics
Acids
Electrons
Water

Keywords

  • co-catalyst
  • cobalt dichalcogenide
  • hydrogen evolution
  • silicon microwire arrays
  • solar water splitting
  • wide range pH toleration

ASJC Scopus subject areas

  • Materials Science(all)

Cite this

Wide Range pH-Tolerable Silicon@Pyrite Cobalt Dichalcogenide Microwire Array Photoelectrodes for Solar Hydrogen Evolution. / Chen, Chih Jung; Yang, Kai Chih; Basu, Mrinmoyee; Lu, Tzu Hsiang; Lu, Ying Rui; Dong, Chung Li; Hu, Shu Fen; Liu, Ru Shi.

In: ACS Applied Materials and Interfaces, Vol. 8, No. 8, 02.03.2016, p. 5400-5407.

Research output: Contribution to journalArticle

Chen, Chih Jung ; Yang, Kai Chih ; Basu, Mrinmoyee ; Lu, Tzu Hsiang ; Lu, Ying Rui ; Dong, Chung Li ; Hu, Shu Fen ; Liu, Ru Shi. / Wide Range pH-Tolerable Silicon@Pyrite Cobalt Dichalcogenide Microwire Array Photoelectrodes for Solar Hydrogen Evolution. In: ACS Applied Materials and Interfaces. 2016 ; Vol. 8, No. 8. pp. 5400-5407.
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abstract = "This study employed silicon@cobalt dichalcogenide microwires (MWs) as wide range pH-tolerable photocathode material for solar water splitting. Silicon microwire arrays were fabricated through lithography and dry etching technologies. Si@Co(OH)2 MWs were utilized as precursors to synthesize Si@CoX2 (X = S or Se) photocathodes. Si@CoS2 and Si@CoSe2 MWs were subsequently prepared by thermal sulfidation and hydrothermal selenization reaction of Si@Co(OH)2, respectively. The CoX2 outer shell served as cocatalyst to accelerate the kinetics of photogenerated electrons from the underlying Si MWs and reduce the recombination. Moreover, the CoX2 layer completely deposited on the Si surface functioned as a passivation layer by decreasing the oxide formation on Si MWs during solar hydrogen evolution. Si@CoS2 photocathode showed a photocurrent density of -3.22 mA cm-2 at 0 V (vs RHE) in 0.5 M sulfuric acid electrolyte, and Si@CoSe2 MWs revealed moderate photocurrent density of -2.55 mA cm-2. However, Si@CoSe2 presented high charge transfer efficiency in neutral and alkaline electrolytes. Continuous chronoamperometry in acid, neutral, and alkaline solutions was conducted at 0 V (vs RHE) to evaluate the photoelectrochemical durability of Si@CoX2 MWs. Si@CoS2 electrode showed no photoresponse after the chronoamperometry test because it was etched through the electrolyte. By contrast, the photocurrent density of Si@CoSe2 MWs gradually increased to -5 mA cm-2 after chronoamperometry characterization owing to the amorphous structure generation.",
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T1 - Wide Range pH-Tolerable Silicon@Pyrite Cobalt Dichalcogenide Microwire Array Photoelectrodes for Solar Hydrogen Evolution

AU - Chen, Chih Jung

AU - Yang, Kai Chih

AU - Basu, Mrinmoyee

AU - Lu, Tzu Hsiang

AU - Lu, Ying Rui

AU - Dong, Chung Li

AU - Hu, Shu Fen

AU - Liu, Ru Shi

PY - 2016/3/2

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N2 - This study employed silicon@cobalt dichalcogenide microwires (MWs) as wide range pH-tolerable photocathode material for solar water splitting. Silicon microwire arrays were fabricated through lithography and dry etching technologies. Si@Co(OH)2 MWs were utilized as precursors to synthesize Si@CoX2 (X = S or Se) photocathodes. Si@CoS2 and Si@CoSe2 MWs were subsequently prepared by thermal sulfidation and hydrothermal selenization reaction of Si@Co(OH)2, respectively. The CoX2 outer shell served as cocatalyst to accelerate the kinetics of photogenerated electrons from the underlying Si MWs and reduce the recombination. Moreover, the CoX2 layer completely deposited on the Si surface functioned as a passivation layer by decreasing the oxide formation on Si MWs during solar hydrogen evolution. Si@CoS2 photocathode showed a photocurrent density of -3.22 mA cm-2 at 0 V (vs RHE) in 0.5 M sulfuric acid electrolyte, and Si@CoSe2 MWs revealed moderate photocurrent density of -2.55 mA cm-2. However, Si@CoSe2 presented high charge transfer efficiency in neutral and alkaline electrolytes. Continuous chronoamperometry in acid, neutral, and alkaline solutions was conducted at 0 V (vs RHE) to evaluate the photoelectrochemical durability of Si@CoX2 MWs. Si@CoS2 electrode showed no photoresponse after the chronoamperometry test because it was etched through the electrolyte. By contrast, the photocurrent density of Si@CoSe2 MWs gradually increased to -5 mA cm-2 after chronoamperometry characterization owing to the amorphous structure generation.

AB - This study employed silicon@cobalt dichalcogenide microwires (MWs) as wide range pH-tolerable photocathode material for solar water splitting. Silicon microwire arrays were fabricated through lithography and dry etching technologies. Si@Co(OH)2 MWs were utilized as precursors to synthesize Si@CoX2 (X = S or Se) photocathodes. Si@CoS2 and Si@CoSe2 MWs were subsequently prepared by thermal sulfidation and hydrothermal selenization reaction of Si@Co(OH)2, respectively. The CoX2 outer shell served as cocatalyst to accelerate the kinetics of photogenerated electrons from the underlying Si MWs and reduce the recombination. Moreover, the CoX2 layer completely deposited on the Si surface functioned as a passivation layer by decreasing the oxide formation on Si MWs during solar hydrogen evolution. Si@CoS2 photocathode showed a photocurrent density of -3.22 mA cm-2 at 0 V (vs RHE) in 0.5 M sulfuric acid electrolyte, and Si@CoSe2 MWs revealed moderate photocurrent density of -2.55 mA cm-2. However, Si@CoSe2 presented high charge transfer efficiency in neutral and alkaline electrolytes. Continuous chronoamperometry in acid, neutral, and alkaline solutions was conducted at 0 V (vs RHE) to evaluate the photoelectrochemical durability of Si@CoX2 MWs. Si@CoS2 electrode showed no photoresponse after the chronoamperometry test because it was etched through the electrolyte. By contrast, the photocurrent density of Si@CoSe2 MWs gradually increased to -5 mA cm-2 after chronoamperometry characterization owing to the amorphous structure generation.

KW - co-catalyst

KW - cobalt dichalcogenide

KW - hydrogen evolution

KW - silicon microwire arrays

KW - solar water splitting

KW - wide range pH toleration

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