preprints.org > chemistry and materials science > electrochemistry > doi: 10.20944/preprints202211.0505.v1

Preprint Article Version 1 Preserved in Portico This version is not peer-reviewed

Version 1 : Received: 26 November 2022 / Approved: 28 November 2022 / Online: 28 November 2022 (08:37:23 CET)

The requirements for efficient replacement of fossil fuel, combined with the growing energy crisis, put hydrogen production into focus. Efficient and cost-effective electrocatalysts are needed for H2 production, and novel strategies for their discovery must be developed. Here we utilized Kinetic Monte Carlo (KMC) simulations to demonstrate that hydrogen evolution reaction (HER) can be boosted via hydrogen spillover to the support when the catalyst surface is largely covered by adsorbed hydrogen under operating conditions. Based on the insights from KMC, we synthesized a series of reduced graphene oxide-supported catalysts and compared their activities towards HER in alkaline media with that of corresponding pure metals. For Ag, Au, and Zn, the support effect is negative, but for Pt, Pd, Fe, Co, and Ni, the presence of the support enhances HER activity. The HER volcano, constructed using calculated hydrogen binding energies and measured HER activities, shows a positive shift of the strong binding branch. This work demonstrates the possibilities of metal|support interface engineering for producing effective HER catalysts and provides general guidelines for choosing novel catalyst-support combinations for electrocatalytic hydrogen production.

hydrogen evolution reaction; hydrogen spillover; interfacial processes; supported catalysts; reduced graphene oxide; Kinetic Monte Carlo; volcano curve; hydrogen adsorption

Chemistry and Materials Science, Electrochemistry

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