Strong Acid-Mediated Proton Transfer via Water Tunneling Fosters Hydrogen Evolution Reaction on MoS2 Derivatives under Alkaline Conditions
Matteo Pugliesi, Giulia Alice Volpato, Ida Ritacco, Giulia Tuci, Mattia Cattelan, Andrea Rossin, Yuefeng Liu, Lucia Caporaso, Matteo Farnesi Camellone, Giuseppe Santoriello, Elena Colusso, Stefano Agnoli, Giuliano Giambastiani
TL;DR
Researchers found that adding acid-ended molecules to MoS2 nanoflakes improves hydrogen production efficiency even in alkaline conditions.
Contribution
The study introduces a pH-insensitive electrocatalyst for hydrogen evolution by enhancing proton transfer via water tunneling.
Findings
Surface-engineered MoS2 with sulfonic-acid groups boosts hydrogen evolution reaction (HER) under alkaline conditions.
Weaker acid groups like benzoic acid do not promote proton transfer via tunneling.
DFT calculations support the role of acidic moieties in water dissociation and tunneling at the surface.
Abstract
The surface functionalization of chemically exfoliated MoS2 (CE-MoS2) nanoflakes with Brønsted-acid end-capped aryl fragments adds an additional level of complexity to the comprehension of the correlation between the electron-donating strength of covalently grafted organic groups (Hammett parameter) and the HER performance of these hybrids. MoS2 nanoflakes decorated with aryl-sulfonic acids promote proton transfer via tunneling of H-species, where weaker benzoic acid groups fail. Thus, surface-engineered CE-MoS2 bearing sulfonic-acid end-capped dangling arms acts as an electrocatalyst that boosts HER kinetics even under an alkaline environment, where water dissociation represents the bottleneck of the process. Density functional theory (DFT) calculations have been used to corroborate experimental evidence and speculate on the role of acidic moieties with respect to water molecule…
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Taxonomy
TopicsMetalloenzymes and iron-sulfur proteins · CO2 Reduction Techniques and Catalysts · Electrocatalysts for Energy Conversion