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

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• 作者：Pedram AbbasiMohammad Asadi ; Cong Liu ; Soroosh Sharifi-Asl ; Baharak SayahpourAmirhossein Behranginia ; Peter ZapolReza Shahbazian-Yassar ; Larry A. Curtiss ; Amin Salehi-Khojin
• 刊名：ACS Nano
• 出版年：2017
• 出版时间：January 24, 2017
• 年：2017
• 卷：11
• 期：1
• 页码：453-460
• 全文大小：504K
• ISSN：1936-086X

文摘

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.