Understanding the degradation of Ag2Cu2O3 electrocatalysts for CO2 reduction†

IF 4.6 3区 材料科学 Q2 CHEMISTRY, MULTIDISCIPLINARY
N. Vorlaufer, J. Josten, A. Hutzler, C. A. Macauley, N. Martić, M. Weiser, G. Schmid, K. J. J. Mayrhofer and P. Felfer
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Abstract

Recently, a mixed-metal oxide with a paramelaconite-type crystal structure (Ag2Cu2O3) has been investigated as a promising catalyst for electrochemical reduction of CO2 and CO. The catalyst operates with a reasonable overpotential and good selectivity. However, during its utilization, the catalyst experiences a degradation in conversion efficiency, thus limiting its potential in industrial application. This has so far been attributed to the unstable nature of the crystal structure, which tends to partition into metallic copper and silver. In this study, we characterized this decomposition using atom probe tomography and analytical electron microscopy. We found this decomposition to take place also under an electron beam without any ongoing reaction conditions. We also found that dissolution mechanisms must play a role in the degradation of the catalyst. This is deduced from the existence of nanostructures which only form during catalyst operation and are comprised of copper and potassium, the latter of which stems from the electrolyte. The composition of these nanostructures was confirmed using an atom probe.

Abstract Image

Ag2Cu2O3电催化剂在CO2还原中的降解研究。
近年来,人们研究了一种具有副乌头状晶体结构的混合金属氧化物(Ag2Cu2O3)作为电化学还原CO2和CO的催化剂,该催化剂具有合理的过电位和良好的选择性。但在使用过程中,催化剂的转化效率下降,限制了其在工业上的应用潜力。到目前为止,这被归因于晶体结构的不稳定性,它倾向于分裂成金属铜和银。在这项研究中,我们使用原子探针断层扫描和分析电子显微镜来表征这种分解。我们发现这种分解在没有任何持续反应条件的电子束下也会发生。我们还发现,溶解机制必须在催化剂的降解中发挥作用。这是由纳米结构的存在推断出来的,这些纳米结构仅在催化剂操作过程中形成,由铜和钾组成,后者来自电解质。用原子探针证实了这些纳米结构的组成。
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来源期刊
Nanoscale Advances
Nanoscale Advances Multiple-
CiteScore
8.00
自引率
2.10%
发文量
461
审稿时长
9 weeks
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