Wawrzyniak Aleksandra, Koper Marc T M
Leiden Institute of Chemistry, Leiden University, Einsteinweg 55, 2333 CC Leiden, The Netherlands.
ACS Catal. 2025 Jan 10;15(3):1514-1521. doi: 10.1021/acscatal.4c05442. eCollection 2025 Feb 7.
Electrochemical carbon dioxide (CO) conversion to value-added, highly reduced chemicals such as methanol (CHOH) is a promising possibility for producing renewable fuel and simultaneous CO recycling. However, this process remains a challenge, with only a few selective electrocatalysts known. Here, we present a study of a palladium monolayer on a platinum (111) single crystal (Pd/Pt(111)) as an electrocatalyst for CO conversion to CHOH. A custom-made setup was employed in order to detect and quantify gaseous and liquid CO reduction products in sufficient concentrations despite the limitations of working with a single-crystalline electrode. Under ambient reaction conditions, a Faradaic efficiency (FE) of 1.5% at -0.9 V vs reversible hydrogen electrode (RHE) was obtained while using CO as the reactant. Other reaction intermediates, carbon monoxide (CO) and formaldehyde (HCHO) were subsequently used as reactants, leading to FEs of 1.8 and 2.5%, respectively, whereas formic acid is not reduced. The corresponding mechanism concluded from our work is compared to the literature. The electrocatalyst introduced here, with a highly well-defined structure for CO conversion to CHOH, opens up possibilities for further catalytic explorations.
将电化学二氧化碳（CO₂）转化为增值的、高度还原的化学品，如甲醇（CH₃OH），是生产可再生燃料和同步回收CO₂的一种很有前景的可能性。然而，这个过程仍然是一个挑战，已知的选择性电催化剂很少。在这里，我们展示了一项关于铂（111）单晶上的钯单层（Pd/Pt(111)）作为将CO₂转化为CH₃OH的电催化剂的研究。尽管使用单晶电极存在局限性，但我们采用了定制装置来检测和定量足够浓度的气态和液态CO₂还原产物。在环境反应条件下，以CO作为反应物时，相对于可逆氢电极（RHE）在-0.9 V时获得了1.5%的法拉第效率（FE）。随后使用其他反应中间体一氧化碳（CO）和甲醛（HCHO）作为反应物，分别导致FE为1.8%和2.5%，而甲酸未被还原。我们从工作中得出的相应机理与文献进行了比较。这里引入的电催化剂具有用于将CO₂转化为CH₃OH的高度明确的结构，为进一步的催化探索开辟了可能性。
