Xu Qiucheng, Joensen Bjørt Óladóttir, Kani Nishithan C, Sartori Andrea, Willson Terry, Varcoe John R, Riillo Luca, Ramunni Anna, Drnec Jakub, Chorkendorff Ib, Seger Brian
Surface Physics and Catalysis (SurfCat) Section, Department of Physics, Technical University of Denmark, Kongens Lyngby, 2800 Kgs., Denmark.
Laboratory of Inorganic Synthesis and Catalysis, Institute of Chemical Sciences and Engineering, Ecole Polytechnique Fédérale de Lausanne (EPFL), Lausanne, CH-1015, Switzerland.
Angew Chem Int Ed Engl. 2025 May 26;64(22):e202501505. doi: 10.1002/anie.202501505. Epub 2025 Mar 27.
Membrane-electrode-assembly (MEA)-based CO electrolysis (COE) has demonstrated the capability to produce C products with high faradaic efficiency at ampere-level current densities. However, most studies on COE have achieved performance benchmarks under strongly alkaline conditions (e.g., ≥1 m KOH, pH ≥14), raising the question of whether such high pH levels are essential for optimal performance. In this study, we investigated the effects of different electrolytes (KHCO, KCO, and KOH) on MEA-based CO electrolysis, focusing on the influence of pH and the impact of anodic oxidation on the selectivity of various liquid products. By adjusting electrolyte concentration and pH, we achieved significant partial current densities for ethanol (189 ± 5 mA cm) and propanol (89 ± 4 mA cm) using 0.5 M KCO. This high performance is attributed to the creation of a moderate local alkaline environment and the relatively high resistance to anodic oxidation. Additionally, durability measurements emphasized the critical importance of eliminating anodic oxidation to optimize MEA-based COE for ethanol and propanol production.
基于膜电极组件(MEA)的CO电解(COE)已证明能够在安培级电流密度下以高法拉第效率生产含碳产物。然而,大多数关于COE的研究都是在强碱性条件下(例如,≥1 M KOH,pH≥14)达到性能基准的,这就引发了一个问题,即如此高的pH值对于最佳性能是否必不可少。在本研究中,我们研究了不同电解质(KHCO₃、K₂CO₃和KOH)对基于MEA的CO电解的影响,重点关注pH值的影响以及阳极氧化对各种液体产物选择性的影响。通过调节电解质浓度和pH值,我们使用0.5 M K₂CO₃实现了乙醇(189±5 mA cm⁻²)和丙醇(89±4 mA cm⁻²)的显著分电流密度。这种高性能归因于形成了适度的局部碱性环境以及对阳极氧化具有相对较高的抗性。此外,耐久性测量强调了消除阳极氧化对于优化基于MEA的COE以生产乙醇和丙醇的至关重要性。