Transition metal sulfide hydrogen evolution catalysts for hydrobromic acid electrolysis

Ivanovskaya, Anna, Singh, Nirala, Liu, Ru-Fen, Kreutzer, Haley, Baltrusaitis, Jonas, Van Nguyen, Trung, Metiu, Horia and McFarland, Eric (2013) Transition metal sulfide hydrogen evolution catalysts for hydrobromic acid electrolysis. Langmuir, 29 1: 480-492. doi:10.1021/la3032489


Author Ivanovskaya, Anna
Singh, Nirala
Liu, Ru-Fen
Kreutzer, Haley
Baltrusaitis, Jonas
Van Nguyen, Trung
Metiu, Horia
McFarland, Eric
Title Transition metal sulfide hydrogen evolution catalysts for hydrobromic acid electrolysis
Journal name Langmuir   Check publisher's open access policy
ISSN 0743-7463
1520-5827
Publication date 2013-01-08
Sub-type Article (original research)
DOI 10.1021/la3032489
Open Access Status
Volume 29
Issue 1
Start page 480
End page 492
Total pages 13
Place of publication Washington, DC, United States
Publisher American Chemical Society
Language eng
Abstract Mixed metal sulfides containing combinations of W, Fe, Mo, Ni, and Ru were synthesized and screened for activity and stability for the hydrogen evolution reaction (HER) in aqueous hydrobromic acid (HBr). Co- and Ni-substituted RuS2 were identified as potentially active HER electrocatalysts by high-throughput screening (HTS), and the specific compositions Co 0.4Ru0.6S2 and Ni0.6Ru 0.4S2 were identified by optimization. Hydrogen evolution activity of Co0.4Ru0.6S2 in HBr is greater than RuS2 or CoS2 and comparable to Pt and commercial Rh xSy. Structural and morphological characterizations of the Co-substituted RuS2 suggest that the nanoparticulate solids are a homogeneous solid solution with a pyrite crystal structure. No phase separation is detected for Co substitutions below 30% by X-ray diffraction. In 0.5 M HBr electrolyte, the Co-Ru electrode material synthesized with 30% Co rapidly lost approximately 34% of the initial loading of Co; thereafter, it was observed to exhibit stable activity for HER with no further loss of Co. Density functional theory calculations indicate that the S2 2- sites are the most important for HER and the presence of Co influences the S2 2- sites such that the hydrogen binding energy at sufficiently high hydrogen coverage is decreased compared to ruthenium sulfide. Although showing high HER activity in a flow cell, the reverse reaction of hydrogen oxidation is slow on the RuS2 catalysts tested when compared to platinum and rhodium sulfide, leaving rhodium sulfide as the only suitable tested material for a regenerative HBr cell due its stability compared to platinum.
Q-Index Code C1
Q-Index Status Provisional Code
Institutional Status Non-UQ

Document type: Journal Article
Sub-type: Article (original research)
Collection: School of Chemical Engineering Publications
 
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