Intriguing H2S Tolerance of the PtRu Alloy for Hydrogen Oxidation Catalysis in PEMFCs : Weakened Pt-S Binding with Slower Adsorption Kinetics
High quality of hydrogen is the key to the long lifetime of proton-exchange membrane fuel cell (PEMFC) vehicles, while trace H2S impurities in hydrogen significantly affect their durability and fuel expense. Herein, we demonstrate a robust PtRu alloy catalyst with an intriguing H2S tolerance as the PEMFC anode, showing a stronger antipoisoning capability toward hydrogen oxidation reaction compared with the Pt/C anode. The PtRu/C-based single PEMFC shows approximately 14.3% loss of cell voltage after 3 h operation with 1 ppm of H2S in hydrogen, significantly lower than that of Pt/C-based PEMFCs (65%). By adopting PtRu/C as the anode, the H2S limit in hydrogen can be increased to 1.7 times that of the Pt/C anode, assuming that the PEMFC runs for 5000 h, which is conductive for the cost reduction of hydrogen purification. The three-electrode electrochemical test indicates that PtRu/C exhibits a slower adsorption kinetics toward S2- species with poisoning rates of 0.02782, 0.02982, and 0.03682 min-1 at temperatures of 25, 35, and 45 °C, respectively, all lower than those of Pt/C. X-ray absorption fine structure spectra indicate the weakened Pt-S binding for PtRu/C in comparison to Pt/C with a longer Pt-S bond length. Density functional theory calculation analyses reveal that adsorption energy of sulfur on the Pt surface was reduced for PtRu/C, showing 1-10% decrease at different Pt sites for (111), (110), and (100) planes, which is ascribed to the downshifted Pt d-band center caused by the ligand and strain effects due to the introduction of second metallic Ru. This work provides a valuable guide for the development of the H2S-tolerant catalysts for long-term application of PEMFCs.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2022 |
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| Erschienen: |
2022 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:14 |
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| Enthalten in: |
ACS applied materials & interfaces - 14(2022), 42 vom: 26. Okt., Seite 47765-47774 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Ke, Shaojie [VerfasserIn] |
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| Links: |
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| Themen: |
Adsorption kinetics |
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| Anmerkungen: |
Date Revised 26.10.2022 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
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| doi: |
10.1021/acsami.2c13742 |
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| funding: |
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| Förderinstitution / Projekttitel: |
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NLM347666922 |
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| 520 | |a High quality of hydrogen is the key to the long lifetime of proton-exchange membrane fuel cell (PEMFC) vehicles, while trace H2S impurities in hydrogen significantly affect their durability and fuel expense. Herein, we demonstrate a robust PtRu alloy catalyst with an intriguing H2S tolerance as the PEMFC anode, showing a stronger antipoisoning capability toward hydrogen oxidation reaction compared with the Pt/C anode. The PtRu/C-based single PEMFC shows approximately 14.3% loss of cell voltage after 3 h operation with 1 ppm of H2S in hydrogen, significantly lower than that of Pt/C-based PEMFCs (65%). By adopting PtRu/C as the anode, the H2S limit in hydrogen can be increased to 1.7 times that of the Pt/C anode, assuming that the PEMFC runs for 5000 h, which is conductive for the cost reduction of hydrogen purification. The three-electrode electrochemical test indicates that PtRu/C exhibits a slower adsorption kinetics toward S2- species with poisoning rates of 0.02782, 0.02982, and 0.03682 min-1 at temperatures of 25, 35, and 45 °C, respectively, all lower than those of Pt/C. X-ray absorption fine structure spectra indicate the weakened Pt-S binding for PtRu/C in comparison to Pt/C with a longer Pt-S bond length. Density functional theory calculation analyses reveal that adsorption energy of sulfur on the Pt surface was reduced for PtRu/C, showing 1-10% decrease at different Pt sites for (111), (110), and (100) planes, which is ascribed to the downshifted Pt d-band center caused by the ligand and strain effects due to the introduction of second metallic Ru. This work provides a valuable guide for the development of the H2S-tolerant catalysts for long-term application of PEMFCs | ||
| 650 | 4 | |a Journal Article | |
| 650 | 4 | |a H2S impurity | |
| 650 | 4 | |a PtRu/C anode | |
| 650 | 4 | |a Pt−S bond | |
| 650 | 4 | |a adsorption kinetics | |
| 650 | 4 | |a hydrogen oxidation reduction | |
| 650 | 4 | |a proton-exchange membrane fuel cells | |
| 700 | 1 | |a Cui, Bolan |e verfasserin |4 aut | |
| 700 | 1 | |a Sun, Chaoyong |e verfasserin |4 aut | |
| 700 | 1 | |a Qin, Yufeng |e verfasserin |4 aut | |
| 700 | 1 | |a Zhang, Jiakun |e verfasserin |4 aut | |
| 700 | 1 | |a Dou, Meiling |e verfasserin |4 aut | |
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