Catalysis Sans Catalyst Loss: The Origins of Prolonged Stability of Graphene–Metal–Graphene Sandwich Architecture for Oxygen Reduction Reactions
Abstract Over the past decades, the design of active catalysts has been the subject of intense research efforts. However, there has been significantly less deliberate emphasis on rationally designing a catalyst system with a prolonged stability. A major obstacle comes from the ambiguity behind how c...
| Main Authors: | , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Wiley
2023-12-01
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| Series: | Advanced Science |
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| Online Access: | https://doi.org/10.1002/advs.202304616 |
| _version_ | 1797401841830461440 |
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| author | Ali Abdelhafiz Ji Il Choi Bote Zhao Jinwon Cho Yong Ding Luke Soule Seung Soon Jang Meilin Liu Faisal M. Alamgir |
| author_facet | Ali Abdelhafiz Ji Il Choi Bote Zhao Jinwon Cho Yong Ding Luke Soule Seung Soon Jang Meilin Liu Faisal M. Alamgir |
| author_sort | Ali Abdelhafiz |
| collection | DOAJ |
| description | Abstract Over the past decades, the design of active catalysts has been the subject of intense research efforts. However, there has been significantly less deliberate emphasis on rationally designing a catalyst system with a prolonged stability. A major obstacle comes from the ambiguity behind how catalyst degrades. Several degradation mechanisms are proposed in literature, but with a lack of systematic studies, the causal relations between degradation and those proposed mechanisms remain ambiguous. Here, a systematic study of a catalyst system comprising of small particles and single atoms of Pt sandwiched between graphene layers, GR/Pt/GR, is studied to unravel the degradation mechanism of the studied electrocatalyst for oxygen reduction reaction(ORR). Catalyst suffers from atomic dissolution under ORR harsh acidic and oxidizing operation voltages. Single atoms trapped in point defects within the top graphene layer on their way hopping through toward the surface of GR/Pt/GR architecture. Trapping mechanism renders individual Pt atoms as single atom catalyst sites catalyzing ORR for thousands of cycles before washed away in the electrolyte. The GR/Pt/GR catalysts also compare favorably to state‐of‐the‐art commercial Pt/C catalysts and demonstrates a rational design of a hybrid nanoarchitecture with a prolonged stability for thousands of operation cycles. |
| first_indexed | 2024-03-09T02:16:08Z |
| format | Article |
| id | doaj.art-bd3c1086712c44108fc8b3c7d88e2d6a |
| institution | Directory Open Access Journal |
| issn | 2198-3844 |
| language | English |
| last_indexed | 2024-03-09T02:16:08Z |
| publishDate | 2023-12-01 |
| publisher | Wiley |
| record_format | Article |
| series | Advanced Science |
| spelling | doaj.art-bd3c1086712c44108fc8b3c7d88e2d6a2023-12-07T04:08:36ZengWileyAdvanced Science2198-38442023-12-011034n/an/a10.1002/advs.202304616Catalysis Sans Catalyst Loss: The Origins of Prolonged Stability of Graphene–Metal–Graphene Sandwich Architecture for Oxygen Reduction ReactionsAli Abdelhafiz0Ji Il Choi1Bote Zhao2Jinwon Cho3Yong Ding4Luke Soule5Seung Soon Jang6Meilin Liu7Faisal M. Alamgir8Department of Nuclear Science and Engineering Massachusetts Institute of Technology 77 Mass Ave Cambridge, MA 02139 USASchool of Materials Science and Engineering Georgia Institute of Technology 771 Ferst Drive Atlanta GA 30332 USASchool of Materials Science and Engineering Georgia Institute of Technology 771 Ferst Drive Atlanta GA 30332 USASchool of Materials Science and Engineering Georgia Institute of Technology 771 Ferst Drive Atlanta GA 30332 USASchool of Materials Science and Engineering Georgia Institute of Technology 771 Ferst Drive Atlanta GA 30332 USASchool of Materials Science and Engineering Georgia Institute of Technology 771 Ferst Drive Atlanta GA 30332 USASchool of Materials Science and Engineering Georgia Institute of Technology 771 Ferst Drive Atlanta GA 30332 USASchool of Materials Science and Engineering Georgia Institute of Technology 771 Ferst Drive Atlanta GA 30332 USASchool of Materials Science and Engineering Georgia Institute of Technology 771 Ferst Drive Atlanta GA 30332 USAAbstract Over the past decades, the design of active catalysts has been the subject of intense research efforts. However, there has been significantly less deliberate emphasis on rationally designing a catalyst system with a prolonged stability. A major obstacle comes from the ambiguity behind how catalyst degrades. Several degradation mechanisms are proposed in literature, but with a lack of systematic studies, the causal relations between degradation and those proposed mechanisms remain ambiguous. Here, a systematic study of a catalyst system comprising of small particles and single atoms of Pt sandwiched between graphene layers, GR/Pt/GR, is studied to unravel the degradation mechanism of the studied electrocatalyst for oxygen reduction reaction(ORR). Catalyst suffers from atomic dissolution under ORR harsh acidic and oxidizing operation voltages. Single atoms trapped in point defects within the top graphene layer on their way hopping through toward the surface of GR/Pt/GR architecture. Trapping mechanism renders individual Pt atoms as single atom catalyst sites catalyzing ORR for thousands of cycles before washed away in the electrolyte. The GR/Pt/GR catalysts also compare favorably to state‐of‐the‐art commercial Pt/C catalysts and demonstrates a rational design of a hybrid nanoarchitecture with a prolonged stability for thousands of operation cycles.https://doi.org/10.1002/advs.202304616catalyst degradation mechanismhybrid catalystoxygen reduction reactionproton exchange membrane fuel cell (PEMFC)graphene |
| spellingShingle | Ali Abdelhafiz Ji Il Choi Bote Zhao Jinwon Cho Yong Ding Luke Soule Seung Soon Jang Meilin Liu Faisal M. Alamgir Catalysis Sans Catalyst Loss: The Origins of Prolonged Stability of Graphene–Metal–Graphene Sandwich Architecture for Oxygen Reduction Reactions Advanced Science catalyst degradation mechanism hybrid catalyst oxygen reduction reaction proton exchange membrane fuel cell (PEMFC) graphene |
| title | Catalysis Sans Catalyst Loss: The Origins of Prolonged Stability of Graphene–Metal–Graphene Sandwich Architecture for Oxygen Reduction Reactions |
| title_full | Catalysis Sans Catalyst Loss: The Origins of Prolonged Stability of Graphene–Metal–Graphene Sandwich Architecture for Oxygen Reduction Reactions |
| title_fullStr | Catalysis Sans Catalyst Loss: The Origins of Prolonged Stability of Graphene–Metal–Graphene Sandwich Architecture for Oxygen Reduction Reactions |
| title_full_unstemmed | Catalysis Sans Catalyst Loss: The Origins of Prolonged Stability of Graphene–Metal–Graphene Sandwich Architecture for Oxygen Reduction Reactions |
| title_short | Catalysis Sans Catalyst Loss: The Origins of Prolonged Stability of Graphene–Metal–Graphene Sandwich Architecture for Oxygen Reduction Reactions |
| title_sort | catalysis sans catalyst loss the origins of prolonged stability of graphene metal graphene sandwich architecture for oxygen reduction reactions |
| topic | catalyst degradation mechanism hybrid catalyst oxygen reduction reaction proton exchange membrane fuel cell (PEMFC) graphene |
| url | https://doi.org/10.1002/advs.202304616 |
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