skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Nanostructured transition metal dichalcogenide electrocatalysts for CO2 reduction in ionic liquid

Abstract

Conversion of carbon dioxide (CO2) into fuels is an attractive solution to many energy and environmental challenges. However, the chemical inertness of CO2 renders many electrochemical and photochemical conversion processes inefficient. We report a transition metal dichalcogenide nanoarchitecture for catalytic electrochemical CO2 conversion to carbon monoxide (CO) in an ionic liquid. We found that tungsten diselenide nanoflakes show a current density of 18.95 milliamperes per square centimeter, CO faradaic efficiency of 24%, and CO formation turnover frequency of 0.28 per second at a low overpotential of 54 millivolts. We also applied this catalyst in a light-harvesting artificial leaf platform that concurrently oxidized water in the absence of any external potential.

Authors:
; ; ; ; ; ; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science - Office of Basic Energy Sciences - Materials Sciences and Engineering Division; National Science Foundation (NSF)
OSTI Identifier:
1352570
DOE Contract Number:
AC02-06CH11357
Resource Type:
Journal Article
Resource Relation:
Journal Name: Science; Journal Volume: 353; Journal Issue: 6298
Country of Publication:
United States
Language:
English

Citation Formats

Asadi, M., Kim, K., Liu, C., Addepalli, A. V., Abbasi, P., Yasaei, P., Phillips, P., Behranginia, A., Cerrato, J. M., Haasch, R., Zapol, P., Kumar, B., Klie, R. F., Abiade, J., Curtiss, L. A., and Salehi-Khojin, A. Nanostructured transition metal dichalcogenide electrocatalysts for CO2 reduction in ionic liquid. United States: N. p., 2016. Web. doi:10.1126/science.aaf4767.
Asadi, M., Kim, K., Liu, C., Addepalli, A. V., Abbasi, P., Yasaei, P., Phillips, P., Behranginia, A., Cerrato, J. M., Haasch, R., Zapol, P., Kumar, B., Klie, R. F., Abiade, J., Curtiss, L. A., & Salehi-Khojin, A. Nanostructured transition metal dichalcogenide electrocatalysts for CO2 reduction in ionic liquid. United States. doi:10.1126/science.aaf4767.
Asadi, M., Kim, K., Liu, C., Addepalli, A. V., Abbasi, P., Yasaei, P., Phillips, P., Behranginia, A., Cerrato, J. M., Haasch, R., Zapol, P., Kumar, B., Klie, R. F., Abiade, J., Curtiss, L. A., and Salehi-Khojin, A. Thu . "Nanostructured transition metal dichalcogenide electrocatalysts for CO2 reduction in ionic liquid". United States. doi:10.1126/science.aaf4767.
@article{osti_1352570,
title = {Nanostructured transition metal dichalcogenide electrocatalysts for CO2 reduction in ionic liquid},
author = {Asadi, M. and Kim, K. and Liu, C. and Addepalli, A. V. and Abbasi, P. and Yasaei, P. and Phillips, P. and Behranginia, A. and Cerrato, J. M. and Haasch, R. and Zapol, P. and Kumar, B. and Klie, R. F. and Abiade, J. and Curtiss, L. A. and Salehi-Khojin, A.},
abstractNote = {Conversion of carbon dioxide (CO2) into fuels is an attractive solution to many energy and environmental challenges. However, the chemical inertness of CO2 renders many electrochemical and photochemical conversion processes inefficient. We report a transition metal dichalcogenide nanoarchitecture for catalytic electrochemical CO2 conversion to carbon monoxide (CO) in an ionic liquid. We found that tungsten diselenide nanoflakes show a current density of 18.95 milliamperes per square centimeter, CO faradaic efficiency of 24%, and CO formation turnover frequency of 0.28 per second at a low overpotential of 54 millivolts. We also applied this catalyst in a light-harvesting artificial leaf platform that concurrently oxidized water in the absence of any external potential.},
doi = {10.1126/science.aaf4767},
journal = {Science},
number = 6298,
volume = 353,
place = {United States},
year = {Thu Jul 28 00:00:00 EDT 2016},
month = {Thu Jul 28 00:00:00 EDT 2016}
}
  • Cited by 81
  • [Pd(triphosphine)(solvent)](BF4)2 complexes have been developed as catalysts for the electrochemical reduction of CO2 to CO. A variety of structural features of these complexes have been varied to determine their effects on the mechanism, rates, and decomposition products of these catalysts. The structural features varied included substituents on the triphosphine ligand, the size of the chelate bite, and donor atoms of the tridentate ligand. Bimetallic catalysts containing two [Pd(triphosphine)(solvent)] units have been prepared and characterized that exhibit a cooperative interaction during CO2 reduction with large rate enhancements compared to their monomeric analogs. As a first step in developing electrocatalysts capable ofmore » reducing CO, electrochemically generated hydrides of Ni and Pd have been shown to transfer their hydride ligands to coordinated CO to form formyl complexes.« less
  • There is an urgent need for the discovery of carbon-neutral sources of energy to avoid the consequences of global warming caused by ever-increasing atmospheric CO{sub 2} levels. An attractive possibility is to use CO{sub 2} captured from industrial emissions as a feedstock for the production of useful fuels and precursors such as carbon monoxide and methanol. An active field of research to achieve this goal is the development of catalysts capable of harnessing solar energy for use in artificial photosynthetic processes for CO{sub 2} reduction. Transition-metal complexes are excellent candidates, and it has already been shown that they can bemore » used to reduce CO{sub 2} with high quantum efficiency. However, they generally suffer from poor visible light absorption, short catalyst lifetimes, and poor reaction rates. In this Perspective, the field of photocatalytic CO{sub 2} reduction is introduced, and recent developments that seek to improve the efficiency of such catalytic processes are highlighted, especially CO{sub 2} reduction with supramolecules and molecular systems in supercritical CO{sub 2} (scCO{sub 2}) or biphasic ionic liquid-scCO{sub 2} mixtures.« less
  • We study the transport properties of monolayer MX{sub 2} (M = Mo, W; X = S, Se, Te) n- and p-channel metal-oxide-semiconductor field effect transistors (MOSFETs) using full-band ballistic non-equilibrium Green's function simulations with an atomistic tight-binding Hamiltonian with hopping potentials obtained from density functional theory. We discuss the subthreshold slope, drain-induced barrier lowering (DIBL), as well as gate-induced drain leakage (GIDL) for different monolayer MX{sub 2} MOSFETs. We also report the possibility of negative differential resistance behavior in the output characteristics of nanoscale monolayer MX{sub 2} MOSFETs.
  • Atomic force microscopy has been used to characterize wear and oxidation of transition metal dichalcogenide surfaces. Sequential images recorded on molybdenum disulfide (MoS{sub 2}) and niobium diselenide (NbSe{sub 2}) surfaces show that wear proceeds at defects, and that MoS{sub 2} wears at least five times more slowly than NbSe{sub 2}. Images of thermally treated MoS{sub 2} and NbSe{sub 2} further demonstrate that oxidation creates surface defects on both materials. However, for similar oxidation conditions, NbSe{sub 2} surfaces show extensive degradation, while MoS{sub 2} surfaces only exhibit isolated defects. The implications of these results to understanding the tribological properties of themore » transition metal dichalcogenides are discussed.« less