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Title: Tailoring the Edge Structure of Molybdenum Disulfide toward Electrocatalytic Reduction of Carbon Dioxide

Abstract

Electrocatalytic conversion of carbon dioxide (CO2) into energy-rich fuels is considered to be the most efficient approach to achieve a carbon neutral cycle. Transition-metal dichalcogenides (TMDCs) have recently shown a very promising catalytic performance for CO2 reduction reaction in an ionic liquid electrolyte. Here, we report that the catalytic performance of molybdenum disulfide (MoS2), a member of TMDCs, can be significantly improved by using an appropriate dopant. Our electrochemical results indicate that 5% niobium (Nb)-doped vertically aligned MoS2 in ionic liquid exhibits 1 order of magnitude higher CO formation turnover frequency (TOF) than pristine MoS2 at an overpotential range of 50-150 mV. The TOF of this catalyst is also 2 orders of magnitude higher than that of Ag nanoparticles over the entire range of studied overpotentials (100-650 mV). Moreover, the in situ differential electrochemical mass spectrometry experiment shows the onset overpotential of 31 mV for this catalyst, which is the lowest onset potential for CO2 reduction reaction reported so far. Our density functional theory calculations reveal that low concentrations of Nb near the Mo edge atoms can enhance the TOF of CO formation by modifying the binding energies of intermediates to MoS2 edge atoms.

Authors:
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Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1352627
DOE Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article
Resource Relation:
Journal Name: ACS Nano; Journal Volume: 11; Journal Issue: 1
Country of Publication:
United States
Language:
English

Citation Formats

Abbasi, Pedram, Asadi, Mohammad, Liu, Cong, Sharifi-Asl, Soroosh, Sayahpour, Baharak, Behranginia, Amirhossein, Zapol, Peter, Shahbazian-Yassar, Reza, Curtiss, Larry A., and Salehi-Khojin, Amin. Tailoring the Edge Structure of Molybdenum Disulfide toward Electrocatalytic Reduction of Carbon Dioxide. United States: N. p., 2017. Web. doi:10.1021/acsnano.6b06392.
Abbasi, Pedram, Asadi, Mohammad, Liu, Cong, Sharifi-Asl, Soroosh, Sayahpour, Baharak, Behranginia, Amirhossein, Zapol, Peter, Shahbazian-Yassar, Reza, Curtiss, Larry A., & Salehi-Khojin, Amin. Tailoring the Edge Structure of Molybdenum Disulfide toward Electrocatalytic Reduction of Carbon Dioxide. United States. doi:10.1021/acsnano.6b06392.
Abbasi, Pedram, Asadi, Mohammad, Liu, Cong, Sharifi-Asl, Soroosh, Sayahpour, Baharak, Behranginia, Amirhossein, Zapol, Peter, Shahbazian-Yassar, Reza, Curtiss, Larry A., and Salehi-Khojin, Amin. Tue . "Tailoring the Edge Structure of Molybdenum Disulfide toward Electrocatalytic Reduction of Carbon Dioxide". United States. doi:10.1021/acsnano.6b06392.
@article{osti_1352627,
title = {Tailoring the Edge Structure of Molybdenum Disulfide toward Electrocatalytic Reduction of Carbon Dioxide},
author = {Abbasi, Pedram and Asadi, Mohammad and Liu, Cong and Sharifi-Asl, Soroosh and Sayahpour, Baharak and Behranginia, Amirhossein and Zapol, Peter and Shahbazian-Yassar, Reza and Curtiss, Larry A. and Salehi-Khojin, Amin},
abstractNote = {Electrocatalytic conversion of carbon dioxide (CO2) into energy-rich fuels is considered to be the most efficient approach to achieve a carbon neutral cycle. Transition-metal dichalcogenides (TMDCs) have recently shown a very promising catalytic performance for CO2 reduction reaction in an ionic liquid electrolyte. Here, we report that the catalytic performance of molybdenum disulfide (MoS2), a member of TMDCs, can be significantly improved by using an appropriate dopant. Our electrochemical results indicate that 5% niobium (Nb)-doped vertically aligned MoS2 in ionic liquid exhibits 1 order of magnitude higher CO formation turnover frequency (TOF) than pristine MoS2 at an overpotential range of 50-150 mV. The TOF of this catalyst is also 2 orders of magnitude higher than that of Ag nanoparticles over the entire range of studied overpotentials (100-650 mV). Moreover, the in situ differential electrochemical mass spectrometry experiment shows the onset overpotential of 31 mV for this catalyst, which is the lowest onset potential for CO2 reduction reaction reported so far. Our density functional theory calculations reveal that low concentrations of Nb near the Mo edge atoms can enhance the TOF of CO formation by modifying the binding energies of intermediates to MoS2 edge atoms.},
doi = {10.1021/acsnano.6b06392},
journal = {ACS Nano},
number = 1,
volume = 11,
place = {United States},
year = {Tue Jan 24 00:00:00 EST 2017},
month = {Tue Jan 24 00:00:00 EST 2017}
}