Breaking the Sabatier Principle by Dynamic Adsorption-Desorption Decoupling in Electrocatalytic Hydrogen Evolution
Year: 2025
Type: preprint
Abstract: 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.
Source: arXiv (Cornell University)
Authors: Yang, Zi-Xuan, Li, Lei, Huang, Tao, Wan, Hui, Wang, X. S., Huang, Gui-Fang, Hu, Wangyu, Huang, Wei-Qing
Language: English
Field: Energy
Domain: Physical Sciences
Open Access status: green
OpenAlex ID: W7091187387
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