Enhancing Hydrogen Evolution Activity of Monolayer Molybdenum Disulfide via a Molecular Proton Mediator

Xiangye Liu, Baichang Li, Fernando A. Soto, Xufan Li, Raymond R. Unocic, Perla B. Balbuena, Avetik R. Harutyunyan, James Hone, Daniel V. Esposito

Research output: Contribution to journalArticlepeer-review

18 Scopus citations


The configuration and local environment of active sites in transition metal dichalcogenides can significantly alter their electrocatalytic activity toward the hydrogen evolution reaction (HER). Herein, we demonstrate that the HER activity of monolayer MoS2electrocatalysts can be enhanced through the modulation of active sites by introducing a molecular mediator that alters the coverage of adsorbed protons. Sodium dodecyl sulfate (SDS) promotes the intrinsic HER activity of both terrace-based sulfur vacancies (VS) and edge sites during HER operation in an acidic environment, leading to increases in the turnover frequency (TOF) of both sites by up to 5 orders of magnitude. Simulations indicate that SDS facilitates proton adsorption by catching protons from hydronium ions and releasing them to VS, which reduces the energy barrier by creating a stair-case-like free energy profile. Our results highlight the ability to tailor the activity of electrocatalysts by synergistically combining proton transfer mediators with engineered active sites.

Original languageEnglish (US)
Pages (from-to)12159-12169
Number of pages11
JournalACS Catalysis
Issue number19
StatePublished - Oct 1 2021

All Science Journal Classification (ASJC) codes

  • Catalysis
  • General Chemistry


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