Electrochemical CO2-to-ethylene conversion on polyamine-incorporated Cu electrodes
Electrochemical CO2-to-ethylene conversion on polyamine-incorporated Cu electrodes
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DOI：
10.1038/s41929-020-00547-0
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发表时间：
2020-12-07
期刊：
影响因子：
37.8
通讯作者：
Gewirth, Andrew A.
中科院分区：
文献类型：
--
作者：
Chen, Xinyi;Chen, Junfeng;Gewirth, Andrew A.
将二氧化碳电化学转化为增值化学品有望实现向碳中和的过渡。然而，由于二氧化碳电还原有多种可能的反应途径，提高特定碳氢化合物产品的选择性具有挑战性。在这里，我们提出了一种通过共电镀开发的铜-多胺杂化催化剂，可显着提高乙烯生产的选择性。与可逆氢电极相比，-0.47 V 下乙烯生产的法拉第效率为 87% +/- 3%，全电池能量效率达到 50% +/- 2%。拉曼测量表明，与夹带很少或不含胺官能团的添加剂相比，夹带在 Cu 电极上的多胺会导致更高的表面 pH 值、更高的 CO 含量和更高的中间体稳定性。更广泛地说，这项工作表明聚合物的掺入可以改变表面反应性并导致在高电流密度下增强产物选择性。
Electrochemical conversion of CO2 into value-added chemicals holds promise to enable the transition to carbon neutrality. Enhancing selectivity for a specific hydrocarbon product is challenging, however, due to numerous possible reaction pathways of CO2 electroreduction. Here we present a Cu-polyamine hybrid catalyst, developed through co-electroplating, that significantly increases the selectivity for ethylene production. The Faradaic efficiency for ethylene production is 87% +/- 3% at -0.47 V versus reversible hydrogen electrode, with full-cell energetic efficiency reaching 50% +/- 2%. Raman measurements indicate that the polyamine entrained on the Cu electrode results in higher surface pH, higher CO content and higher stabilization of intermediates compared with entrainment of additives containing little or no amine functionality. More broadly, this work shows that polymer incorporation can alter surface reactivity and lead to enhanced product selectivity at high current densities.