Pinning effect of lattice Pb suppressing lattice oxygen reactivity of Pb-RuO2 enables stable industrial-level electrolysis
Abstract Ruthenium (Ru) is widely recognized as a low-cost alternative to iridium as anode electrocatalyst in proton-exchange membrane water electrolyzers (PEMWE). However, the reported Ru-based catalysts usually only operate within tens of hours in PEMWE because of their intrinsically high reactivi...
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Nature Portfolio
2024-11-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-024-53905-y |
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| author | Chenhui Zhou Lu Li Zhaoqi Dong Fan Lv Hongyu Guo Kai Wang Menggang Li Zhengyi Qian Na Ye Zheng Lin Mingchuan Luo Shaojun Guo |
| author_facet | Chenhui Zhou Lu Li Zhaoqi Dong Fan Lv Hongyu Guo Kai Wang Menggang Li Zhengyi Qian Na Ye Zheng Lin Mingchuan Luo Shaojun Guo |
| author_sort | Chenhui Zhou |
| collection | DOAJ |
| description | Abstract Ruthenium (Ru) is widely recognized as a low-cost alternative to iridium as anode electrocatalyst in proton-exchange membrane water electrolyzers (PEMWE). However, the reported Ru-based catalysts usually only operate within tens of hours in PEMWE because of their intrinsically high reactivity of lattice oxygen that leads to irrepressible Ru leaching and structural collapse. Herein, we report a design concept by employing large-sized and acid-resistant lattice lead (Pb) as a second element to induce a pinning effect for effectively narrowing the moving channels of oxygen atoms, thereby lowering the reactivity of lattice oxygen in Ru oxides. The Pb-RuO2 catalyst presents a low overpotential of 188 ± 2 mV at 10 mA cm−2 and can sustain for over 1100 h in an acid medium with a negligible degradation rate of 19 μV h−1. Particularly, the Pb-RuO2-based PEMWE can operate for more than 250 h at 500 mA cm−2 with a low degradation rate of only 17 μV h−1. Experimental and theoretical calculation results reveal that Ru-O covalency is reduced due to the unique 6s−2p−4d orbital hybridization, which increases the loss energy of lattice oxygen and suppresses the over-oxidation of Ru for improved long-term stability in PEMWE. |
| format | Article |
| id | doaj-art-9240d69ff1044dc786122d3e3fdf2ddb |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2024-11-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-9240d69ff1044dc786122d3e3fdf2ddb2024-11-17T12:37:31ZengNature PortfolioNature Communications2041-17232024-11-011511910.1038/s41467-024-53905-yPinning effect of lattice Pb suppressing lattice oxygen reactivity of Pb-RuO2 enables stable industrial-level electrolysisChenhui Zhou0Lu Li1Zhaoqi Dong2Fan Lv3Hongyu Guo4Kai Wang5Menggang Li6Zhengyi Qian7Na Ye8Zheng Lin9Mingchuan Luo10Shaojun Guo11School of Materials Science and Engineering, Peking UniversitySchool of Materials Science and Engineering, Peking UniversitySchool of Materials Science and Engineering, Peking UniversitySchool of Materials Science and Engineering, Peking UniversitySchool of Materials Science and Engineering, Peking UniversitySchool of Materials Science and Engineering, Peking UniversitySchool of Materials Science and Engineering, Peking UniversitySchool of Materials Science and Engineering, Peking UniversitySchool of Materials Science and Engineering, Peking UniversitySchool of Materials Science and Engineering, Peking UniversitySchool of Materials Science and Engineering, Peking UniversitySchool of Materials Science and Engineering, Peking UniversityAbstract Ruthenium (Ru) is widely recognized as a low-cost alternative to iridium as anode electrocatalyst in proton-exchange membrane water electrolyzers (PEMWE). However, the reported Ru-based catalysts usually only operate within tens of hours in PEMWE because of their intrinsically high reactivity of lattice oxygen that leads to irrepressible Ru leaching and structural collapse. Herein, we report a design concept by employing large-sized and acid-resistant lattice lead (Pb) as a second element to induce a pinning effect for effectively narrowing the moving channels of oxygen atoms, thereby lowering the reactivity of lattice oxygen in Ru oxides. The Pb-RuO2 catalyst presents a low overpotential of 188 ± 2 mV at 10 mA cm−2 and can sustain for over 1100 h in an acid medium with a negligible degradation rate of 19 μV h−1. Particularly, the Pb-RuO2-based PEMWE can operate for more than 250 h at 500 mA cm−2 with a low degradation rate of only 17 μV h−1. Experimental and theoretical calculation results reveal that Ru-O covalency is reduced due to the unique 6s−2p−4d orbital hybridization, which increases the loss energy of lattice oxygen and suppresses the over-oxidation of Ru for improved long-term stability in PEMWE.https://doi.org/10.1038/s41467-024-53905-y |
| spellingShingle | Chenhui Zhou Lu Li Zhaoqi Dong Fan Lv Hongyu Guo Kai Wang Menggang Li Zhengyi Qian Na Ye Zheng Lin Mingchuan Luo Shaojun Guo Pinning effect of lattice Pb suppressing lattice oxygen reactivity of Pb-RuO2 enables stable industrial-level electrolysis Nature Communications |
| title | Pinning effect of lattice Pb suppressing lattice oxygen reactivity of Pb-RuO2 enables stable industrial-level electrolysis |
| title_full | Pinning effect of lattice Pb suppressing lattice oxygen reactivity of Pb-RuO2 enables stable industrial-level electrolysis |
| title_fullStr | Pinning effect of lattice Pb suppressing lattice oxygen reactivity of Pb-RuO2 enables stable industrial-level electrolysis |
| title_full_unstemmed | Pinning effect of lattice Pb suppressing lattice oxygen reactivity of Pb-RuO2 enables stable industrial-level electrolysis |
| title_short | Pinning effect of lattice Pb suppressing lattice oxygen reactivity of Pb-RuO2 enables stable industrial-level electrolysis |
| title_sort | pinning effect of lattice pb suppressing lattice oxygen reactivity of pb ruo2 enables stable industrial level electrolysis |
| url | https://doi.org/10.1038/s41467-024-53905-y |
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