Highly selective plasma-activated copper catalysts for carbon dioxide reduction to ethylene.
Highly selective plasma-activated copper catalysts for carbon dioxide reduction to ethylene.
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DOI：
10.1038/ncomms12123
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发表时间：
2016-06-30
影响因子：
16.6
通讯作者：
Cuenya BR
中科院分区：
文献类型：
--
作者：
Mistry H;Varela AS;Bonifacio CS;Zegkinoglou I;Sinev I;Choi YW;Kisslinger K;Stach EA;Yang JC;Strasser P;Cuenya BR
迫切需要开发利用可再生能源将二氧化碳等废物转化为碳氢燃料的技术。二氧化碳可以在铜催化剂上电化学还原为烃，尽管需要更高的效率。我们已经开发出氧化铜催化剂，通过简单和可调的等离子体处理，显示出较低的二氧化碳电还原过电位和对乙烯的选择性（60%）。在此，我们通过将电化学测量与显微镜和光谱表征技术相结合，深入了解这些催化剂的改进性能。操作X射线吸收光谱和横截面扫描透射电子显微镜显示，氧化铜是令人惊讶的耐还原和铜+物种在反应过程中保持在表面上。我们的研究结果表明，氧化物衍生的铜催化剂的粗糙度在确定催化性能中仅起部分作用，而铜+的存在是降低起始电位和提高乙烯选择性的关键。 二氧化碳电还原是一种很有前途的烃类合成方法，但需要更高效和选择性更高的催化剂。在这里，作者表明，等离子体活化的铜可以催化二氧化碳还原为乙烯，具有高效率，并揭示阳离子铜作为活性中心。
There is an urgent need to develop technologies that use renewable energy to convert waste products such as carbon dioxide into hydrocarbon fuels. Carbon dioxide can be electrochemically reduced to hydrocarbons over copper catalysts, although higher efficiency is required. We have developed oxidized copper catalysts displaying lower overpotentials for carbon dioxide electroreduction and record selectivity towards ethylene (60%) through facile and tunable plasma treatments. Herein we provide insight into the improved performance of these catalysts by combining electrochemical measurements with microscopic and spectroscopic characterization techniques. Operando X-ray absorption spectroscopy and cross-sectional scanning transmission electron microscopy show that copper oxides are surprisingly resistant to reduction and copper+ species remain on the surface during the reaction. Our results demonstrate that the roughness of oxide-derived copper catalysts plays only a partial role in determining the catalytic performance, while the presence of copper+ is key for lowering the onset potential and enhancing ethylene selectivity. Carbon dioxide electroreduction is a promising route to hydrocarbon synthesis, but more efficient and selective catalysts are needed. Here the authors show that plasma-activated copper can catalyse the reduction of carbon dioxide to ethylene with high efficiency and reveal cationic copper as the active site.