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Highly Active and Stable Hybrid Catalyst of Cobalt-Doped FeS2 Nanosheets–Carbon Nanotubes for Hydrogen Evolution Reaction
- Wang, Di-Yan, Gong, Ming, Chou, Hung-Lung, Pan, Chun-Jern, Chen, Hsin-An, Wu, Yingpeng, Lin, Meng-Chang, Guan, Mingyun, Yang, Jiang, Chen, Chun-Wei, Wang, Yuh-Lin, Hwang, Bing-Joe, Chen, Chia-Chun, Dai, Hongjie
- Journal of the American Chemical Society 2015 v.137 no.4 pp. 1587-1592
- X-ray diffraction, adsorption, carbon nanotubes, catalysts, catalytic activity, clean energy, cobalt, cost effectiveness, durability, electrochemistry, hydrogen production, iron, nanosheets, platinum, pyrite, spectroscopy
- 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 ∼0.12 V at 20 mA/cm², small Tafel slope of ∼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 (∼7 mg/cm²). 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.