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Low‐Coordinated Edge Sites on Ultrathin Palladium Nanosheets Boost Carbon Dioxide Electroreduction Performance
Authors:Wenjin Zhu  Lei Zhang  Piaoping Yang  Congling Hu  Zhibin Luo  Xiaoxia Chang  Prof Dr Zhi‐Jian Zhao  Prof Dr Jinlong Gong
Institution:Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Collaborative Innovation Center of Chemical Science and Engineering, Tianjin University, Tianjin, China
Abstract:Electrochemical conversion of carbon dioxide (CO2) to value‐added products is a possible way to decrease the problems resulting from CO2 emission. Thanks to the eminent conductivity and proper adsorption to intermediates, Pd has become a promising candidate for CO2 electroreduction (CO2ER). However, Pd‐based nanocatalysts generally need a large overpotential. Herein we describe that ultrathin Pd nanosheets effectively reduce the onset potential for CO by exposing abundant atoms with comparatively low generalized coordination number. Hexagonal Pd nanosheets with 5 atomic thickness and 5.1 nm edge length reached CO faradaic efficiency of 94 % at ?0.5 V, without any decay after a stability test of 8 h. It appears to be the most efficient among all of Pd‐based catalysts toward CO2ER. Uniform hexagonal morphology made it reasonable to build models and take DFT calculations. The enhanced activity originates from mainly edge sites on palladium nanosheets.
Keywords:CO2 electrochemical reduction  generalized coordination number  low-coordinate sites  palladium  nanosheets
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