Breaking the Sabatier Principle by Dynamic Adsorption-Desorption Decoupling in Electrocatalytic Hydrogen Evolution
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arXiv
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| Format: | Preprint |
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2025
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| author | Yang, Zi-Xuan Li, Lei Huang, Tao Wan, Hui Wang, X. S. Huang, Gui-Fang Hu, Wangyu Huang, Wei-Qing |
| author_facet | Yang, Zi-Xuan Li, Lei Huang, Tao Wan, Hui Wang, X. S. Huang, Gui-Fang Hu, Wangyu Huang, Wei-Qing |
| contents | The Sabatier principle establishes a fundamental trade-off in heterogeneous electrocatalysis.In the hydrogen evolution reaction (HER), this trade-off is manifested by the coupling of Volmer step, which requires strong hydrogen adsorption, with the Heyrovsky/Tafel step, which favors facile desorption, thus giving rise to the classical volcano relationship and limiting activity even at $ΔG=0$. Here, we demonstrate a ferroelectric platform with dynamic tunability -- monolayer GeS$_2$ decorated with transition metal atoms as a proof-of-concept -- where polarization-driven surface electronic reconstruction enables real-time modulation of intermediate binding strength, thereby breaking the Sabatier constraint. Reversible control of hydrogen adsorption allows strong H binding to accelerate the Volmer step, followed by weakened adsorption to promote the Heyrovsky/Tafel step.This dynamic adsorption-desorption decoupling not only surpasses the volcano limit to achieve unprecedented HER activity, but also establishes a general paradigm for designing adaptive electrocatalysts capable of reconfiguring under operating conditions. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2510_10555 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Breaking the Sabatier Principle by Dynamic Adsorption-Desorption Decoupling in Electrocatalytic Hydrogen Evolution Yang, Zi-Xuan Li, Lei Huang, Tao Wan, Hui Wang, X. S. Huang, Gui-Fang Hu, Wangyu Huang, Wei-Qing Materials Science The Sabatier principle establishes a fundamental trade-off in heterogeneous electrocatalysis.In the hydrogen evolution reaction (HER), this trade-off is manifested by the coupling of Volmer step, which requires strong hydrogen adsorption, with the Heyrovsky/Tafel step, which favors facile desorption, thus giving rise to the classical volcano relationship and limiting activity even at $ΔG=0$. Here, we demonstrate a ferroelectric platform with dynamic tunability -- monolayer GeS$_2$ decorated with transition metal atoms as a proof-of-concept -- where polarization-driven surface electronic reconstruction enables real-time modulation of intermediate binding strength, thereby breaking the Sabatier constraint. Reversible control of hydrogen adsorption allows strong H binding to accelerate the Volmer step, followed by weakened adsorption to promote the Heyrovsky/Tafel step.This dynamic adsorption-desorption decoupling not only surpasses the volcano limit to achieve unprecedented HER activity, but also establishes a general paradigm for designing adaptive electrocatalysts capable of reconfiguring under operating conditions. |
| title | Breaking the Sabatier Principle by Dynamic Adsorption-Desorption Decoupling in Electrocatalytic Hydrogen Evolution |
| topic | Materials Science |
| url | https://arxiv.org/abs/2510.10555 |