Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 137, Issue 4, Pages 1587-1592Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja511572q
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Funding
- Stanford GCEP, a Steinhart/Reed Award from Stanford Precourt Institute for Energy
- DOE
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Hydrogen evolution reaction (HER) from water through electrocatalysis using cost-effective materials to replace precious Pt catalysts holds great promise for clean energy technologies. In this work we developed a highly active and stable catalyst containing Co doped earth abundant iron pyrite FeS2 nanosheets hybridized with carbon nanotubes (Fe1-xCoxS2/CNT hybrid catalysts) for HER in acidic solutions. The pyrite phase of Fe1-xCoxS2/CNT was characterized by powder X-ray diffraction and absorption spectroscopy. Electrochemical measurements showed a low overpotential of similar to 0.12 V at 20 mA/cm(2), small Tafel slope of similar to 46 mV/decade, and long-term durability over 40 h of HER operation using bulk quantities of Fe0.9Co0.1S2/CNT hybrid catalysts at high loadings (similar to 7 mg/cm(2)). Density functional theory calculation revealed that the origin of high catalytic activity stemmed from a large reduction of the kinetic energy barrier of H atom adsorption on FeS2 surface upon Co doping in the iron pyrite structure. It is also found that the high HER catalytic activity of Fe0.9Co0.1S2 hinges on the hybridization with CNTs to impart strong heteroatomic interactions between CNT and Fe0.9Co0.1S2. This work produces the most active HER catalyst based on iron pyrite, suggesting a scalable, low cost, and highly efficient catalyst for hydrogen generation.
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