Unconventional p–d Hybridization Interaction in PtGa Ultrathin Nanowires Boosts Oxygen Reduction Electrocatalysis
Alloying 3d transition metals with Pt has been discovered as an effective strategy to boost the catalytic activity in oxygen reduction reaction (ORR), which, however, often raises the insufficient catalyst durability issue due to rapid leaching of the 3d metal elements. To overcome this issue and re...
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| Published in | Journal of the American Chemical Society Vol. 141; no. 45; pp. 18083 - 18090 |
|---|---|
| Main Authors | , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
United States
American Chemical Society
13.11.2019
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| Subjects | |
| Online Access | Get full text |
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| Abstract | Alloying 3d transition metals with Pt has been discovered as an effective strategy to boost the catalytic activity in oxygen reduction reaction (ORR), which, however, often raises the insufficient catalyst durability issue due to rapid leaching of the 3d metal elements. To overcome this issue and realize enhancements in both the activity and the durability properties, here we report a new catalytic structure based on PtGa ultrathin alloy nanowires (NWs), which feature an unconventional strong p–d hybridization interaction. Relative to commercial Pt catalyst, the optimum Pt4.31Ga NWs catalyst exhibited 10.5- and 12.1-fold enhancement in the ORR mass activity and specific activity, respectively. Particularly, the Pt4.31Ga NWs catalyst showed only 15.8% loss in the mass activity after 30 000 cycles of durability test, as compared to a big decrease of 79.6% for the commercial Pt catalyst. Our mechanistic studies find a strong p–d hybridization interaction between Ga and Pt that accounts for the improved ORR performance via synergistically optimizing the surface electronic structure, enhancing the oxidation resistance of Pt, and suppressing the leaching of lattice Ga. We believe this work provides new perspectives to design active and durable electrocatalysts toward ORR. |
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| AbstractList | Alloying 3d transition metals with Pt has been discovered as an effective strategy to boost the catalytic activity in oxygen reduction reaction (ORR), which, however, often raises the insufficient catalyst durability issue due to rapid leaching of the 3d metal elements. To overcome this issue and realize enhancements in both the activity and the durability properties, here we report a new catalytic structure based on PtGa ultrathin alloy nanowires (NWs), which feature an unconventional strong p-d hybridization interaction. Relative to commercial Pt catalyst, the optimum Pt4.31Ga NWs catalyst exhibited 10.5- and 12.1-fold enhancement in the ORR mass activity and specific activity, respectively. Particularly, the Pt4.31Ga NWs catalyst showed only 15.8% loss in the mass activity after 30 000 cycles of durability test, as compared to a big decrease of 79.6% for the commercial Pt catalyst. Our mechanistic studies find a strong p-d hybridization interaction between Ga and Pt that accounts for the improved ORR performance via synergistically optimizing the surface electronic structure, enhancing the oxidation resistance of Pt, and suppressing the leaching of lattice Ga. We believe this work provides new perspectives to design active and durable electrocatalysts toward ORR.Alloying 3d transition metals with Pt has been discovered as an effective strategy to boost the catalytic activity in oxygen reduction reaction (ORR), which, however, often raises the insufficient catalyst durability issue due to rapid leaching of the 3d metal elements. To overcome this issue and realize enhancements in both the activity and the durability properties, here we report a new catalytic structure based on PtGa ultrathin alloy nanowires (NWs), which feature an unconventional strong p-d hybridization interaction. Relative to commercial Pt catalyst, the optimum Pt4.31Ga NWs catalyst exhibited 10.5- and 12.1-fold enhancement in the ORR mass activity and specific activity, respectively. Particularly, the Pt4.31Ga NWs catalyst showed only 15.8% loss in the mass activity after 30 000 cycles of durability test, as compared to a big decrease of 79.6% for the commercial Pt catalyst. Our mechanistic studies find a strong p-d hybridization interaction between Ga and Pt that accounts for the improved ORR performance via synergistically optimizing the surface electronic structure, enhancing the oxidation resistance of Pt, and suppressing the leaching of lattice Ga. We believe this work provides new perspectives to design active and durable electrocatalysts toward ORR. Alloying 3d transition metals with Pt has been discovered as an effective strategy to boost the catalytic activity in oxygen reduction reaction (ORR), which, however, often raises the insufficient catalyst durability issue due to rapid leaching of the 3d metal elements. To overcome this issue and realize enhancements in both the activity and the durability properties, here we report a new catalytic structure based on PtGa ultrathin alloy nanowires (NWs), which feature an unconventional strong p–d hybridization interaction. Relative to commercial Pt catalyst, the optimum Pt₄.₃₁Ga NWs catalyst exhibited 10.5- and 12.1-fold enhancement in the ORR mass activity and specific activity, respectively. Particularly, the Pt₄.₃₁Ga NWs catalyst showed only 15.8% loss in the mass activity after 30 000 cycles of durability test, as compared to a big decrease of 79.6% for the commercial Pt catalyst. Our mechanistic studies find a strong p–d hybridization interaction between Ga and Pt that accounts for the improved ORR performance via synergistically optimizing the surface electronic structure, enhancing the oxidation resistance of Pt, and suppressing the leaching of lattice Ga. We believe this work provides new perspectives to design active and durable electrocatalysts toward ORR. Alloying 3d transition metals with Pt has been discovered as an effective strategy to boost the catalytic activity in oxygen reduction reaction (ORR), which, however, often raises the insufficient catalyst durability issue due to rapid leaching of the 3d metal elements. To overcome this issue and realize enhancements in both the activity and the durability properties, here we report a new catalytic structure based on PtGa ultrathin alloy nanowires (NWs), which feature an unconventional strong p–d hybridization interaction. Relative to commercial Pt catalyst, the optimum Pt4.31Ga NWs catalyst exhibited 10.5- and 12.1-fold enhancement in the ORR mass activity and specific activity, respectively. Particularly, the Pt4.31Ga NWs catalyst showed only 15.8% loss in the mass activity after 30 000 cycles of durability test, as compared to a big decrease of 79.6% for the commercial Pt catalyst. Our mechanistic studies find a strong p–d hybridization interaction between Ga and Pt that accounts for the improved ORR performance via synergistically optimizing the surface electronic structure, enhancing the oxidation resistance of Pt, and suppressing the leaching of lattice Ga. We believe this work provides new perspectives to design active and durable electrocatalysts toward ORR. Alloying 3d transition metals with Pt has been discovered as an effective strategy to boost the catalytic activity in oxygen reduction reaction (ORR), which, however, often raises the insufficient catalyst durability issue due to rapid leaching of the 3d metal elements. To overcome this issue and realize enhancements in both the activity and the durability properties, here we report a new catalytic structure based on PtGa ultrathin alloy nanowires (NWs), which feature an unconventional strong p-d hybridization interaction. Relative to commercial Pt catalyst, the optimum Pt Ga NWs catalyst exhibited 10.5- and 12.1-fold enhancement in the ORR mass activity and specific activity, respectively. Particularly, the Pt Ga NWs catalyst showed only 15.8% loss in the mass activity after 30 000 cycles of durability test, as compared to a big decrease of 79.6% for the commercial Pt catalyst. Our mechanistic studies find a strong p-d hybridization interaction between Ga and Pt that accounts for the improved ORR performance via synergistically optimizing the surface electronic structure, enhancing the oxidation resistance of Pt, and suppressing the leaching of lattice Ga. We believe this work provides new perspectives to design active and durable electrocatalysts toward ORR. |
| Author | Gao, Lei Pan, Anlian Li, Xingxing Ma, Chao Lu, Shanfu Yang, Jinlong Lu, Yangfan Peng, Zhenmeng Huang, Hongwen Yao, Zhaoyu Bai, Huijuan |
| AuthorAffiliation | Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics State Key Lab of Silicon Materials, School of Materials Science and Engineering Beijing Key Laboratory of Bio-inspired Energy Materials and Devices, School of Space and Environment College of Materials Science and Engineering Department of Chemical and Biomolecular Engineering Zhejiang University |
| AuthorAffiliation_xml | – name: Zhejiang University – name: State Key Lab of Silicon Materials, School of Materials Science and Engineering – name: College of Materials Science and Engineering – name: Department of Chemical and Biomolecular Engineering – name: Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics – name: Beijing Key Laboratory of Bio-inspired Energy Materials and Devices, School of Space and Environment |
| Author_xml | – sequence: 1 givenname: Lei surname: Gao fullname: Gao, Lei organization: College of Materials Science and Engineering – sequence: 2 givenname: Xingxing surname: Li fullname: Li, Xingxing organization: Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics – sequence: 3 givenname: Zhaoyu surname: Yao fullname: Yao, Zhaoyu organization: College of Materials Science and Engineering – sequence: 4 givenname: Huijuan surname: Bai fullname: Bai, Huijuan organization: Beijing Key Laboratory of Bio-inspired Energy Materials and Devices, School of Space and Environment – sequence: 5 givenname: Yangfan surname: Lu fullname: Lu, Yangfan organization: Zhejiang University – sequence: 6 givenname: Chao orcidid: 0000-0001-8599-9340 surname: Ma fullname: Ma, Chao organization: College of Materials Science and Engineering – sequence: 7 givenname: Shanfu orcidid: 0000-0001-9873-6654 surname: Lu fullname: Lu, Shanfu organization: Beijing Key Laboratory of Bio-inspired Energy Materials and Devices, School of Space and Environment – sequence: 8 givenname: Zhenmeng orcidid: 0000-0003-1230-6800 surname: Peng fullname: Peng, Zhenmeng email: zpeng@uakron.edu organization: Department of Chemical and Biomolecular Engineering – sequence: 9 givenname: Jinlong orcidid: 0000-0002-5651-5340 surname: Yang fullname: Yang, Jinlong organization: Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics – sequence: 10 givenname: Anlian orcidid: 0000-0003-3335-3067 surname: Pan fullname: Pan, Anlian organization: College of Materials Science and Engineering – sequence: 11 givenname: Hongwen orcidid: 0000-0003-3967-6182 surname: Huang fullname: Huang, Hongwen email: huanghw@hnu.edu.cn organization: Zhejiang University |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/31639295$$D View this record in MEDLINE/PubMed |
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| Snippet | Alloying 3d transition metals with Pt has been discovered as an effective strategy to boost the catalytic activity in oxygen reduction reaction (ORR), which,... |
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| SubjectTerms | alloys catalysts catalytic activity durability electrochemistry nanowires oxidation oxygen platinum |
| Title | Unconventional p–d Hybridization Interaction in PtGa Ultrathin Nanowires Boosts Oxygen Reduction Electrocatalysis |
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