Low-Coordinated Edge Sites on Ultrathin Palladium Nanosheets Boost Carbon Dioxide Electroreduction Performance
Low-Coordinated Edge Sites on Ultrathin Palladium Nanosheets Boost Carbon Dioxide Electroreduction Performance
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超薄钯纳米片上的低配位边缘位点可提高二氧化碳电还原性能
DOI：
10.1002/anie.201806432
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发表时间：
2018
期刊：
影响因子：
--
通讯作者：
Gong Jinlong
中科院分区：
文献类型：
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作者：
Zhu Wenjin;Zhang Lei;Yang Piaoping;Hu Congling;Luo Zhibin;Chang Xiaoxia;Zhao Zhi-Jian;Gong Jinlong
将二氧化碳（CO2）电化学转化为附加值产品是减少CO2排放问题的一种可能途径。由于Pd具有良好的导电性和对中间体的良好吸附性，使其成为CO2电还原反应的理想催化剂。然而，基于Pd的纳米催化剂通常需要大的过电位。在本文中，我们描述了双金属Pd纳米片通过暴露具有相对低的广义配位数的丰富原子来有效地降低CO的起始电势。具有5个原子厚度和5.1 nm边长的半导体Pd纳米片在-0.5 V下达到94%的CO法拉第效率，在8小时的稳定性测试后没有任何衰减。 它似乎是所有Pd基催化剂中对CO2 ER最有效的。均匀的六边形形貌使得建立模型和进行DFT计算是合理的。增强的活性主要来源于钯纳米片上的边缘位点。
Electrochemical conversion of carbon dioxide (CO2) to value‐added products is a possible way to decrease the problems resulting from CO2emission. Thanks to the eminent conductivity and proper adsorption to intermediates, Pd has become a promising candidate for CO2electroreduction (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.