Stability of supported Pd-based ethanol oxidation reaction electrocatalysts in alkaline media

IF 6.5 1区化学 Q2 CHEMISTRY, PHYSICAL Journal of Catalysis Pub Date : 2024-10-21 DOI:10.1016/j.jcat.2024.115816

Tuani C. Gentil , Maria Minichova , Valentín Briega-Martos , Victor S. Pinheiro , Felipe M. Souza , João Paulo C. Moura , Júlio César M. Silva , Bruno L. Batista , Mauro C. Santos , Serhiy Cherevko

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Abstract

This study evaluates the dissolution of the supported electrocatalysts Pd/C, PdSn/C, PdNb/C, and PdFe₃O₄/C during ethanol oxidation reaction for Alkaline Direct Liquid Fuel Cells (ADLFC) applications. A scanning flow cell (SFC) combined to an inductively coupled plasma mass spectrometry (online ICP-MS) is used to assess the dissolution stability in a broad potential window. Accelerated stress tests with and without ethanol are developed using a rotating disk electrode (RDE) with dissolution products analysis by ex-situ ICP-MS. Potential profiles simulating those experienced by the catalyst during regular fuel cell operation were used. Sn and Fe catalysts demonstrate improved activity and stability compared with the material with Pd alone. For these reasons, PdSn/C and PdFe₃O₄/C are suitable for ADLFC applications. Severe Nb dissolution destabilizes Pd, increasing its leaching. This work demonstrates that while additional metals and oxides can improve the alcohol oxidation kinetics of Pd, these additives’ dissolution stability must already be considered at the catalyst design stage.

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碱性介质中支撑型钯基乙醇氧化反应电催化剂的稳定性

本研究评估了 ADLFC 应用中乙醇氧化反应过程中支撑电催化剂 Pd/C、PdSn/C、PdNb/C 和 PdFe3O4/C 的溶解情况。扫描流动池（SFC）与电感耦合质谱仪（在线 ICP-MS）相结合，用于评估宽电位窗口中的溶解稳定性。使用旋转盘电极（RDE）开发了含乙醇和不含乙醇的加速应力测试，并通过原位 ICP-MS 分析溶解产物。使用的电位曲线模拟了催化剂在燃料电池正常运行期间所经历的电位曲线。与单独使用钯的材料相比，锡和铁催化剂的活性和稳定性都有所提高。因此，PdSn/C 和 PdFe3O4/C 适用于 ADLFC 应用。严重的铌溶解会破坏钯的稳定性，增加钯的沥滤。这项工作表明，虽然添加金属和氧化物可以改善钯的醇氧化动力学，但在催化剂设计阶段就必须考虑这些添加剂的溶解稳定性。

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来源期刊

Journal of Catalysis 工程技术-工程：化工

CiteScore

12.30

自引率

5.50%

发文量

447

审稿时长

31 days

期刊介绍： The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes. The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods. The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.