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1.Tailoring the Edge Structure of Molybdenum Disulfide toward Electrocatalytic Reduction of Carbon Dioxide
机构:Pedram Abbasi† , Mohammad Asadi†, Cong Liu‡, Soroosh Sharifi-Asl† , Baharak Sayahpour† , Amirhossein Behranginia†, Peter Zapol‡ , Reza Shahbazian-Yassar†, Larry A. Curtiss‡, and Amin Salehi-Khojin*† † Departmentof Mechanical and Industrial Engineering, University of Illinois at Chicago, Chicago, Illinois 60607, United States‡ MaterialsScience Division, Argonne National Laboratory, Argonne, Illinois 60439, United States
关键词:atomic doping; CO2 reduction reaction; electrocatalysis; ionic liquid; transition-metal dichalcogenides;
摘要: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.
年:2017
出版单位:ACS Nano
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