Rare earth evoked subsurface oxygen species in platinum alloy catalysts enable durable fuel cells
Alleviating the degradation issue of Pt based alloy catalysts, thereby simultaneously achieving high mass activity and high durability in proton exchange membrane fuel cells (PEMFCs), is highly challenging. Herein, we provide a new paradigm to address this issue via delaying the place exchange betwe...
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sg-ntu-dr.10356-1761132024-05-13T07:29:54Z Rare earth evoked subsurface oxygen species in platinum alloy catalysts enable durable fuel cells Yang, Liting Bai, Jingsen Zhang, Nanshu Jiang, Zheng Wang, Ying Xiao, Meiling Liu, Changpeng Zhu, Siyuan Xu, Jason Zhichuan Ge, Junjie Xing, Wei School of Materials Science and Engineering Engineering Fuel Cells Oxygen Reduction Reaction; Alleviating the degradation issue of Pt based alloy catalysts, thereby simultaneously achieving high mass activity and high durability in proton exchange membrane fuel cells (PEMFCs), is highly challenging. Herein, we provide a new paradigm to address this issue via delaying the place exchange between adsorbed oxygen species and surface Pt atoms, thereby inhibiting Pt dissolution, through introducing rare earth bonded subsurface oxygen atoms. We have succeeded in introducing Gd-O dipoles into Pt3 Ni via a high temperature entropy-driven process, with direct spectral evidence attained from both soft and hard X-ray absorption spectroscopies. The higher rated power of 0.93 W cm-2 and superior current density of 562.2 mA cm-2 at 0.8 V than DOE target for heavy-duty vehicles in H2 -air mode suggest the great potential of Gd-O-Pt3 Ni towards practical application in heavy-duty transportation. Moreover, the mass activity retention (1.04 A mgPt -1 ) after 40 k cycles accelerated durability tests is even 2.4 times of the initial mass activity goal for DOE 2025 (0.44 A mgPt -1 ), due to the weakened Pt-Oads bond interaction and the delayed place exchange process, via repulsive forces between surface O atoms and those in the sublayer. This work addresses the critical roadblocks to the widespread adoption of PEMFCs. Thank the National Natural Science Foundation of China (22272160, 22373097), the Jilin Province Science and Technology Development Program (YDZJ202202CXJD011, 20210502002ZP, 20220101056JC), Dalian National Laboratory for Clean Energy (DNL), CAS, the Research Innovation Fund (grant DNL202010) for financial support. 2024-05-13T07:29:54Z 2024-05-13T07:29:54Z 2024 Journal Article Yang, L., Bai, J., Zhang, N., Jiang, Z., Wang, Y., Xiao, M., Liu, C., Zhu, S., Xu, J. Z., Ge, J. & Xing, W. (2024). Rare earth evoked subsurface oxygen species in platinum alloy catalysts enable durable fuel cells. Angewandte Chemie International Edition, 63(7), e202315119-. https://dx.doi.org/10.1002/anie.202315119 1433-7851 https://hdl.handle.net/10356/176113 10.1002/anie.202315119 38129317 2-s2.0-85181879143 7 63 e202315119 en Angewandte Chemie International Edition © 2023 Wiley-VCH GmbH. All rights reserved. |
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Engineering Fuel Cells Oxygen Reduction Reaction; |
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Engineering Fuel Cells Oxygen Reduction Reaction; Yang, Liting Bai, Jingsen Zhang, Nanshu Jiang, Zheng Wang, Ying Xiao, Meiling Liu, Changpeng Zhu, Siyuan Xu, Jason Zhichuan Ge, Junjie Xing, Wei Rare earth evoked subsurface oxygen species in platinum alloy catalysts enable durable fuel cells |
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Alleviating the degradation issue of Pt based alloy catalysts, thereby simultaneously achieving high mass activity and high durability in proton exchange membrane fuel cells (PEMFCs), is highly challenging. Herein, we provide a new paradigm to address this issue via delaying the place exchange between adsorbed oxygen species and surface Pt atoms, thereby inhibiting Pt dissolution, through introducing rare earth bonded subsurface oxygen atoms. We have succeeded in introducing Gd-O dipoles into Pt3 Ni via a high temperature entropy-driven process, with direct spectral evidence attained from both soft and hard X-ray absorption spectroscopies. The higher rated power of 0.93 W cm-2 and superior current density of 562.2 mA cm-2 at 0.8 V than DOE target for heavy-duty vehicles in H2 -air mode suggest the great potential of Gd-O-Pt3 Ni towards practical application in heavy-duty transportation. Moreover, the mass activity retention (1.04 A mgPt -1 ) after 40 k cycles accelerated durability tests is even 2.4 times of the initial mass activity goal for DOE 2025 (0.44 A mgPt -1 ), due to the weakened Pt-Oads bond interaction and the delayed place exchange process, via repulsive forces between surface O atoms and those in the sublayer. This work addresses the critical roadblocks to the widespread adoption of PEMFCs. |
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School of Materials Science and Engineering |
author_facet |
School of Materials Science and Engineering Yang, Liting Bai, Jingsen Zhang, Nanshu Jiang, Zheng Wang, Ying Xiao, Meiling Liu, Changpeng Zhu, Siyuan Xu, Jason Zhichuan Ge, Junjie Xing, Wei |
format |
Article |
author |
Yang, Liting Bai, Jingsen Zhang, Nanshu Jiang, Zheng Wang, Ying Xiao, Meiling Liu, Changpeng Zhu, Siyuan Xu, Jason Zhichuan Ge, Junjie Xing, Wei |
author_sort |
Yang, Liting |
title |
Rare earth evoked subsurface oxygen species in platinum alloy catalysts enable durable fuel cells |
title_short |
Rare earth evoked subsurface oxygen species in platinum alloy catalysts enable durable fuel cells |
title_full |
Rare earth evoked subsurface oxygen species in platinum alloy catalysts enable durable fuel cells |
title_fullStr |
Rare earth evoked subsurface oxygen species in platinum alloy catalysts enable durable fuel cells |
title_full_unstemmed |
Rare earth evoked subsurface oxygen species in platinum alloy catalysts enable durable fuel cells |
title_sort |
rare earth evoked subsurface oxygen species in platinum alloy catalysts enable durable fuel cells |
publishDate |
2024 |
url |
https://hdl.handle.net/10356/176113 |
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1800916165094014976 |