Rabiee Hesamoddin, Dutta Abhijit, Yan Penghui, Ge Lei, Dorosti Fatereh, Yu Xin, Rieder Alain, Broekmann Peter
Department of Chemistry, Biochemistry and Pharmaceutical Sciences, University of Bern, Freiestrasse 3, Bern, 3012, Switzerland.
NCCR Catalysis, University of Bern, Freiestrasse 3, Bern, 3012, Switzerland.
Angew Chem Int Ed Engl. 2025 Aug 14:e202513103. doi: 10.1002/anie.202513103.
The electrochemical CO reduction reaction (ECOR) offers a promising pathway to convert CO into value-added products. While catalyst advances remain crucial, gas-diffusion electrodes (GDEs) architecture is equally vital in CO electrolyzer design. Most ECOR studies use pure CO feeds, whereas industrial sources like flue gas contain ∼15% CO, requiring costly purification. Eliminating this step demands electrolyzers that directly process impure streams via in situ separation. Here, we introduce a composite GDE (CGDE) featuring a thin CO-selective interlayer of intrinsically microporous polymer (PIM-1) reinforced with the CO-philic ionic liquid [Emim][BF]. This layer selectively adsorbs CO and suppresses N/O existence at the catalyst interface. In simulated flue gas (15% CO, 5% O in N), the CGDE with 20 wt% [Emim][BF]/PIM-1 achieved >70% CO Faradaic efficiency (FE) at 100 mA cm , versus ∼20% FE for a pristine GDE. Multiphysics simulations confirmed effective CO delivery through the selective layer, with minimal O permeation. Cost estimation analysis indicates around 25% reduction in CO's minimum selling price using the integrated design and >50% under ideal performance metrics by eliminating compression/transport. These results demonstrate that advanced electrode design with CO-selective interlayer enables direct mixed-gas ECOR, establishes key design criteria for selective layers, and significantly improves process economics.
电化学CO还原反应（ECOR）为将CO转化为高附加值产品提供了一条有前景的途径。虽然催化剂的进步仍然至关重要，但气体扩散电极（GDE）结构在CO电解槽设计中同样至关重要。大多数ECOR研究使用纯CO进料，而像烟道气这样的工业来源含有约15%的CO，需要昂贵的净化处理。要消除这一步骤，就需要能够通过原位分离直接处理不纯物流的电解槽。在此，我们介绍一种复合气体扩散电极（CGDE），其具有由亲CO离子液体[Emim][BF]增强的固有微孔聚合物（PIM-1）的薄CO选择性中间层。该层选择性吸附CO并抑制催化剂界面处N/O的存在。在模拟烟道气（15% CO，N2中5% O2）中，含有20 wt% [Emim][BF]/PIM-1的CGDE在100 mA cm-2时实现了>70%的CO法拉第效率（FE），而原始GDE的FE约为20%。多物理场模拟证实了通过选择性层的有效CO传输，且O2渗透极少。成本估算分析表明，使用集成设计，CO的最低销售价格降低约25%，在理想性能指标下通过消除压缩/运输可降低>50%。这些结果表明，具有CO选择性中间层的先进电极设计能够实现直接混合气体ECOR，确立了选择性层的关键设计标准，并显著提高了工艺经济性。
