Fe–Sn–N–C Catalysts: Advancing Oxygen Reduction Reaction Performance

催化作用 氧还原反应 氧气 化学 还原(数学) 有机化学 电化学 物理化学 几何学 数学 电极
作者
Julia Buschermöhle,Julia Müller‐Hülstede,Henrike Schmies,Dana Schonvogel,Tanja Zierdt,Rene Lucka,Franz Renz,Peter Wagner,Michael Wark
出处
期刊:ACS Catalysis [American Chemical Society]
卷期号:15 (6): 4477-4488 被引量:30
标识
DOI:10.1021/acscatal.4c06338
摘要

High-temperature proton exchange membrane fuel cells (HT-PEMFCs) typically rely on platinum-based catalysts, which require high loadings due to Pt deactivation by phosphates from the phosphoric acid-doped membrane. As alternative catalysts for the oxygen reduction reaction, metal–nitrogen-carbons (M–N–Cs) are promising due to their high intrinsic activity and tolerance to phosphates. However, low volumetric activity compared to Pt nanoparticles on carbon blacks (Pt/C) and insufficient stability limit their applicability. In order to enhance the stability and activity of Fe–N–Cs, this study investigates the incorporation of tin as a second metal, resulting in Fe–Sn–N–Cs, prepared by a metal–organic framework (MOF)-based approach. Stable and highly active catalysts with total mass activities of 8.2 A g–1 (Fe–Sn–N–C (1:1)) and 19.3 A g–1 (Fe–Sn–N–C (1:0.3)) in 0.5 mol L–1 H3PO4, drastically exceeding those of the commercial Fe–N–C catalyst PMF-014401 (Pajarito-Powder, 4.8 A g–1), are obtained by a synthesis without the need for subsequent purification steps. A stress test under harsh conditions (0.6–1.0 VRHE, 10,000 cycles, O2-saturated electrolyte) ascertains stability-enhancing effects of tin, highlighting an increase in stability in conjunction with the tin content. These results provide a valuable contribution to the development of cost-effective HT-PEMFCs by significantly enhancing the catalytic activity of platinum group metal-free catalysts.
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