Julia G. Buschermöhle, Julia Müller-Hülstede, Henrike Schmies, Dana Schonvogel, Tanja Zierdt, Rene Lucka, Franz Renz, Peter Wagner, Michael Wark
{"title":"Fe-Sn-N-C 催化剂:提高氧还原反应性能","authors":"Julia G. Buschermöhle, Julia Müller-Hülstede, Henrike Schmies, Dana Schonvogel, Tanja Zierdt, Rene Lucka, Franz Renz, Peter Wagner, Michael Wark","doi":"10.1021/acscatal.4c06338","DOIUrl":null,"url":null,"abstract":"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<sup>–1</sup> (Fe–Sn–N–C (1:1)) and 19.3 A g<sup>–1</sup> (Fe–Sn–N–C (1:0.3)) in 0.5 mol L<sup>–1</sup> H<sub>3</sub>PO<sub>4</sub>, drastically exceeding those of the commercial Fe–N–C catalyst PMF-014401 (Pajarito-Powder, 4.8 A g<sup>–1</sup>), are obtained by a synthesis without the need for subsequent purification steps. A stress test under harsh conditions (0.6–1.0 V<sub>RHE</sub>, 10,000 cycles, O<sub>2</sub>-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.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"34 1","pages":""},"PeriodicalIF":11.3000,"publicationDate":"2025-03-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Fe–Sn–N–C Catalysts: Advancing Oxygen Reduction Reaction Performance\",\"authors\":\"Julia G. Buschermöhle, Julia Müller-Hülstede, Henrike Schmies, Dana Schonvogel, Tanja Zierdt, Rene Lucka, Franz Renz, Peter Wagner, Michael Wark\",\"doi\":\"10.1021/acscatal.4c06338\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"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<sup>–1</sup> (Fe–Sn–N–C (1:1)) and 19.3 A g<sup>–1</sup> (Fe–Sn–N–C (1:0.3)) in 0.5 mol L<sup>–1</sup> H<sub>3</sub>PO<sub>4</sub>, drastically exceeding those of the commercial Fe–N–C catalyst PMF-014401 (Pajarito-Powder, 4.8 A g<sup>–1</sup>), are obtained by a synthesis without the need for subsequent purification steps. A stress test under harsh conditions (0.6–1.0 V<sub>RHE</sub>, 10,000 cycles, O<sub>2</sub>-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.\",\"PeriodicalId\":9,\"journal\":{\"name\":\"ACS Catalysis \",\"volume\":\"34 1\",\"pages\":\"\"},\"PeriodicalIF\":11.3000,\"publicationDate\":\"2025-03-02\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Catalysis \",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1021/acscatal.4c06338\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Catalysis ","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acscatal.4c06338","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
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.
期刊介绍:
ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels.
The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.