Membrane-controlled CO 2 electrocatalysts with switchable C2 product selectivity and high faradaic efficiency for ethanol
Membrane-controlled CO 2 electrocatalysts with switchable C2 product selectivity and high faradaic efficiency for ethanol
复制标题
具有可切换 C2 产品选择性和乙醇高法拉第效率的膜控制 CO 2 电催化剂
DOI：
10.1039/d3ta00613a
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发表时间：
2023
影响因子：
11.9
通讯作者：
Barile, Christopher J.
中科院分区：
文献类型：
--
作者：
Akter, Tania;Barile, Christopher J.
双金属铜材料是有前景的二氧化碳还原电催化剂，可用于形成有价值的多碳产品。我们描述了膜改性的 Ag-Cu 电催化剂，可以高选择性地将 CO2 转化为 C2 产品。虽然传统的 Ag-Cu 催化剂产生乙烯 (C2H4) 作为主要产物，但我们证明，通过引入质子可渗透的含氟聚合物，可以将产物选择性转换为乙醇 (C2H5OH)。通过优化催化剂成分、电压、膜厚度和特性，我们开发了一种能够产生 C2H5OH 的催化剂，其法拉第效率高达 72%，使其成为报道的 C2H5OH 选择性最高的 Ag-Cu 催化剂。最后，我们讨论了详细的化学机制，解释了膜覆盖层的疏水性如何使催化剂具有可切换的 C2 产物选择性。
Bimetallic Cu materials are promising CO2 reduction electrocatalysts for the formation of valuable multicarbon products. We describe membrane-modified Ag–Cu electrocatalysts that convert CO2 to C2 products with high selectivity. While traditional Ag–Cu catalysts generate ethylene (C2H4) as the main product, we demonstrate that product selectivity can be switched to ethanol (C2H5OH) by introducing a proton-permeable fluoropolymer. By optimizing the catalyst composition, voltage, and membrane thickness and identity, we develop a catalyst that generates C2H5OH with up to 72% faradaic efficiency, making it the most selective Ag–Cu catalyst for C2H5OH reported. Lastly, we discuss a detailed chemical mechanism that explains how the hydrophobicity of the membrane overlayer enables catalysts with switchable C2 product selectivity.