Abstract
The optimization of traditional electrocatalysts has reached a point where progress is impeded by fundamental physical factors including inherent scaling relations among thermokinetic characteristics of different elementary reaction steps, non-Nernstian behavior, and electronic structure of the catalyst. This indicates that the currently utilized classes of electrocatalysts may not be adequate for future needs. This study reports on synthesis and characterization of a new class of materials based on 2D transition metal dichalcogenides including sulfides, selenides, and tellurides of group V and VI transition metals that exhibit excellent catalytic performance for both oxygen reduction and evolution reactions in an aprotic medium with Li salts. The reaction rates are much higher for these materials than previously reported catalysts for these reactions. The reasons for the high activity are found to be the metal edges with adiabatic electron transfer capability and a cocatalyst effect involving an ionic-liquid electrolyte. These new materials are expected to have high activity for other core electrocatalytic reactions and open the way for advances in energy storage and catalysis.
| Original language | English |
|---|---|
| Article number | 1804453 |
| Journal | Advanced Materials |
| Volume | 31 |
| Issue number | 4 |
| DOIs | |
| State | Published - Jan 25 2019 |
| Externally published | Yes |
Funding
The work of A.S.-K., R.F.K., L.M., P.Y., Z.H., X.H., P.A., and B.S. was supported by the National Science Foundation DMREF Grant 1729420. X.H. and R.F.K. also acknowledge funding from the National Science Foundation (Grant No. DMR-0959470, DMR-1626065) for the acquisition of the UIC JEOL JEMARM200CF with the Gatan Quantum GIF EELS spectrometer. The work at Washington University (J.C., S.B.C., and R.M.) was supported through NSF DMREF Grant 1729787. This work used the computational resources of the Extreme Science and Engineering Discovery Environment (XSEDE), which was supported by National Science Foundation grant number ACI-1053575, Bebop, a high-performance computing cluster operated by the Laboratory Computing Resource Center at Argonne National Laboratory, and the National Energy Research Scientific Computing Center (NERSC). The work of A.S.-K., R.F.K., L.M., P.Y., Z.H., X.H., P.A., and B.S. was supported by the National Science Foundation DMREF Grant 1729420. X.H. and R.F.K. also acknowledge funding from the National Science Foundation (Grant No. DMR-0959470, DMR-1626065) for the acquisition of the UIC JEOL JEMARM200CF with the Gatan Quantum GIF EELS spectrometer. The work at Washington University (J.C., S.B.C., and R.M.) was supported through NSF DMREF Grant 1729787. This work used the computational resources of the Extreme Science and Engineering Discovery Environment (XSEDE), which was supported by National Science Foundation grant number ACI-1053575, Bebop, a high-performance computing cluster operated by the Laboratory Computing Resource Center at Argonne National Laboratory, and the National Energy Research Scientific Computing Center (NERSC). The work of F.K.-A. and S.F. was supported by the National Science Foundation (Grant No. EFRI-1542864) and University of Illinois Work by P.Z. and L.A.C. was supported by the US Department of Energy, BES Materials Sciences under Contract DEAC02-06CH11357 with UChicago Argonne, LLC, operator of Argonne National Laboratory. Work by L.C. was supported by supported by the Joint Center for Energy Storage Research (JCESR), an Energy Innovation Hub funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences. The work of J.G. was supported through a Department of Energy award through the Office of Science, Office of Basic Energy Sciences, Chemical, Biological, and Geosciences Division, under award number DE-SC0010379. R.E.W. acknowledges support from the U.S. Department of Energy, Office of Science, Office of Workforce Development for Teachers and Scientists, Office of Science Graduate Student Research (SCGSR) Program. The SCGSR program is administered by the Oak Ridge Institute for Science and Education (ORISE) for the DOE. ORISE is managed by ORAU under contract number DE-SC0014664. M.V. was supported by Laboratory Directed Research and Development (LDRD) funding from Argonne National Laboratory, provided by the Director, Office of Science, of the U.S. Department of Energy under Contract No. DE-AC02-06CH11357. The authors thank Dr. Xinqi Chen at Atomic and Nanoscale Characterization Experimental Center (NUANCE) in Northwestern University for helpful guidance and discussions.
Keywords
- electrocatalysis
- ionic liquids
- oxygen evolution reaction
- oxygen reduction reaction
- transition metal dichalcogenides