2D High-Entropy Transition Metal Dichalcogenides for Carbon Dioxide Electrocatalysis

John Cavin, Alireza Ahmadiparidari, Leily Majidi, Arashdeep Singh Thind, Saurabh N. Misal, Aditya Prajapati, Zahra Hemmat, Sina Rastegar, Andrew Beukelman, Meenesh R. Singh, Kinga A. Unocic, Amin Salehi-Khojin, Rohan Mishra

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124 Scopus citations

Abstract

High-entropy alloys combine multiple principal elements at a near equal fraction to form vast compositional spaces to achieve outstanding functionalities that are absent in alloys with one or two principal elements. Here, the prediction, synthesis, and multiscale characterization of 2D high-entropy transition metal dichalcogenide (TMDC) alloys with four/five transition metals is reported. Of these, the electrochemical performance of a five-component alloy with the highest configurational entropy, (MoWVNbTa)S2, is investigated for CO2 conversion to CO, revealing an excellent current density of 0.51 A cm−2 and a turnover frequency of 58.3 s−1 at ≈ −0.8 V versus reversible hydrogen electrode. First-principles calculations show that the superior CO2 electroreduction is due to a multi-site catalysis wherein the atomic-scale disorder optimizes the rate-limiting step of CO desorption by facilitating isolated transition metal edge sites with weak CO binding. 2D high-entropy TMDC alloys provide a materials platform to design superior catalysts for many electrochemical systems.

Original languageEnglish
Article number2100347
JournalAdvanced Materials
Volume33
Issue number31
DOIs
StatePublished - Aug 5 2021

Funding

This work was supported by National Science Foundation (NSF) DMREF 1729420 and NSF‐CBET 1800357 (A.AP, S.M., Z.H., A.S.‐K.) and NSF CBET 1729787 (J.C., A.B., and R.M.). A.S.T. was supported by NSF DMR‐1806147. R.M. further acknowledges partial support through NSF DMR‐1809571. A portion of the STEM experiments was conducted at the Center for Nanophase Materials Sciences at Oak Ridge National Laboratory, which is a Department of Energy (DOE) Office of Science User Facility, through a user project. STEM‐EDS microscopy research was supported by the Office of Nuclear Energy, Fuel Cycle R&D Program and the Nuclear Science User Facilities. This work used the computational resources of the Extreme Science and Engineering Discovery Environment (XSEDE), which is supported by NSF ACI‐1548562. The authors would also like to acknowledge NUANCE at Northwestern University for their resources. This work was supported by National Science Foundation (NSF) DMREF 1729420 and NSF-CBET 1800357 (A.AP, S.M., Z.H., A.S.-K.) and NSF CBET 1729787 (J.C., A.B., and R.M.). A.S.T. was supported by NSF DMR-1806147. R.M. further acknowledges partial support through NSF DMR-1809571. A portion of the STEM experiments was conducted at the Center for Nanophase Materials Sciences at Oak Ridge National Laboratory, which is a Department of Energy (DOE) Office of Science User Facility, through a user project. STEM-EDS microscopy research was supported by the Office of Nuclear Energy, Fuel Cycle R&D Program and the Nuclear Science User Facilities. This work used the computational resources of the Extreme Science and Engineering Discovery Environment (XSEDE), which is supported by NSF ACI-1548562. The authors would also like to acknowledge NUANCE at Northwestern University for their resources.

Keywords

  • 2D materials
  • electrocatalysis
  • high entropy alloys
  • transition metal dichalcogenides

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