Ma Ming, Kim Sangkuk, Chorkendorff Ib, Seger Brian
Surface Physics and Catalysis (SurfCat) Section, Department of Physics, Technical University of Denmark 2800 Kgs. Lyngby Denmark
Surface Chemistry Laboratory of Energy/Electronic Materials (SCHEMA), Department of Chemical Engineering, Pohang University of Science and Technology Pohang 37673 Korea.
Chem Sci. 2020 Aug 3;11(33):8854-8861. doi: 10.1039/d0sc03047c.
In this work, the effect of ion-selective membranes on the detailed carbon balance was systematically analyzed for high-rate CO reduction in GDE-type flow electrolyzers. By using different ion-selective membranes, we show nearly identical catalytic selectivity for CO reduction, which is primarily due to a similar local reaction environment created at the cathode/electrolyte interface the introduction of a catholyte layer. In addition, based on a systematic exploration of gases released from electrolytes and the dynamic change of electrolyte speciation, we demonstrate the explicit discrepancy in carbon balance paths for the captured CO at the cathode/catholyte interface reaction with OH when using different ion-selective membranes: (i) the captured CO could be transported through an anion exchange membrane in the form of CO , subsequently releasing CO along with O in the anolyte, and (ii) with a cation exchange membrane, the captured CO would be accumulated in the catholyte in the form of CO , while (iii) with the use of a bipolar membrane, the captured CO could be released at the catholyte/membrane interface in the form of gaseous CO. The unique carbon balance path for each type of membrane is linked to ion species transported through the membranes.
在这项工作中,针对GDE型流动电解槽中高速率CO还原,系统分析了离子选择膜对详细碳平衡的影响。通过使用不同的离子选择膜,我们展示了对CO还原几乎相同的催化选择性,这主要归因于在阴极/电解质界面通过引入阴极电解液层所创造的相似局部反应环境。此外,基于对电解质释放气体的系统探索以及电解质形态的动态变化,我们证明了在阴极/阴极电解液界面使用不同离子选择膜时,捕获的CO在碳平衡路径上存在明显差异:与OH反应时,(i)捕获的CO可以以CO的形式通过阴离子交换膜传输,随后在阳极电解液中与O一起释放出CO;(ii)使用阳离子交换膜时,捕获的CO将以CO的形式在阴极电解液中积累;而(iii)使用双极膜时,捕获的CO可以以气态CO的形式在阴极电解液/膜界面释放。每种类型膜独特的碳平衡路径与通过膜传输的离子种类相关。