The edges of 2D materials have emerged as promising electrochemical catalyst systems, yet their performance still lags behind that of noble metals. Here, we demonstrate the potential of oriented electric fields (OEFs) to enhance the electrochemical activity of 2D materials edges. By atomically engineering the edge of a fluorographene/graphene/MoS2 heterojunction nanoribbon, strong and localized OEFs were realized as confirmed by simulations and spatially resolved spectroscopy. The observed fringing OEF results in an enhancement of the heterogeneous charge transfer rate between the edge and the electrolyte by 2 orders of magnitude according to impedance spectroscopy. Ab initio calculations indicate a field-induced decrease in the reactant adsorption energy as the origin of this improvement. We apply the OEF-enhanced edge reactivity to hydrogen evolution reactions (HER) and observe a significantly enhanced electrochemical performance, as evidenced by a 30% decrease in Tafel slope and a 3-fold enhanced turnover frequency. Our findings demonstrate the potential of OEFs for tailoring the catalytic properties of 2D material edges toward future complex reactions.

Department of Low Dimensional Systems J Heyrovský Institute of Physical Chemistry Prague 18200 Czech Republic

Department of Physics National Taiwan University Taipei 10617 Taiwan

Institute of Atomic and Molecular Sciences Academia Sinica Taipei 10617 Taiwan

International Graduate Program of Molecular Science and Technology National Taiwan University Taipei 10617 Taiwan

Molecular Science and Technology Program Taiwan International Graduate Program Academia Sinica Taipei 10617 Taiwan

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