08 January 2024 | Zhi Wen Chen, Jian Li, Pengfei Ou, Jianan Erick Huang, Zi Wen, Li Xin Chen, Xue Yao, Guang Ming Cai, Chun Cheng Yang, Chandra Veer Singh, Qing Jiang
The Sabatier principle, a widely explored concept in heterogeneous catalysis, suggests that the optimal activity for a catalytic reaction occurs when the adsorption energy of the reactant is neither too weak nor too strong. However, achieving this "just right" adsorption energy often results in a peak in catalytic activity, beyond which further improvements are challenging. This study introduces an unusual Sabatier principle for high entropy alloy (HEA) catalysts in the hydrogen evolution reaction (HER). Through density functional theory (DFT) calculations, the authors discovered that HEA surfaces exhibit spatially varying adsorption free energies of H+ (ΔG_H+), following a Gaussian distribution. This distribution allows for a larger σ value and a μ value closer to 0 eV, which enhances the catalytic activity for HER. A PtFeCoNiCu HEA catalyst was synthesized, showing superior HER performance with an overpotential of 10.8 mV at -10 mA cm⁻² and 4.6 times higher intrinsic activity compared to state-of-the-art Pt/C. The unusual Sabatier principle is also extended to other adsorbents (C+, O+, and N+) on HEA surfaces, indicating its potential for various catalytic reactions.The Sabatier principle, a widely explored concept in heterogeneous catalysis, suggests that the optimal activity for a catalytic reaction occurs when the adsorption energy of the reactant is neither too weak nor too strong. However, achieving this "just right" adsorption energy often results in a peak in catalytic activity, beyond which further improvements are challenging. This study introduces an unusual Sabatier principle for high entropy alloy (HEA) catalysts in the hydrogen evolution reaction (HER). Through density functional theory (DFT) calculations, the authors discovered that HEA surfaces exhibit spatially varying adsorption free energies of H+ (ΔG_H+), following a Gaussian distribution. This distribution allows for a larger σ value and a μ value closer to 0 eV, which enhances the catalytic activity for HER. A PtFeCoNiCu HEA catalyst was synthesized, showing superior HER performance with an overpotential of 10.8 mV at -10 mA cm⁻² and 4.6 times higher intrinsic activity compared to state-of-the-art Pt/C. The unusual Sabatier principle is also extended to other adsorbents (C+, O+, and N+) on HEA surfaces, indicating its potential for various catalytic reactions.