Synergy of compress strain and antioxidant of platinum-copper for enhanced the oxygen reduction performance
The development of efficient and durable electrocatalysts for oxygen reduction reaction (ORR) holds a pivotal significance in the successful commercialization of proton exchange membrane fuel cells (PEMFCs) but is still challenging. Herein, we report a worm-liked PtCu nanocrystals dispersed on nitro...
| Main Authors: | , , , , , , , , , , , |
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| Other Authors: | |
| Format: | Journal Article |
| Language: | English |
| Published: |
2024
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| Subjects: | |
| Online Access: | https://hdl.handle.net/10356/178560 |
| _version_ | 1824455346584813568 |
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| author | Zhang, Jun Liang, Pingjuan Xu, Xinlan Wang, Rong Liu, Shuyue Wang, Chunyuan Liu, Boyu Luo, Laizheng Jin, Meng Liu, Huan Yi, Huan Lu, Shi-Yu |
| author2 | School of Physical and Mathematical Sciences |
| author_facet | School of Physical and Mathematical Sciences Zhang, Jun Liang, Pingjuan Xu, Xinlan Wang, Rong Liu, Shuyue Wang, Chunyuan Liu, Boyu Luo, Laizheng Jin, Meng Liu, Huan Yi, Huan Lu, Shi-Yu |
| author_sort | Zhang, Jun |
| collection | NTU |
| description | The development of efficient and durable electrocatalysts for oxygen reduction reaction (ORR) holds a pivotal significance in the successful commercialization of proton exchange membrane fuel cells (PEMFCs) but is still challenging. Herein, we report a worm-liked PtCu nanocrystals dispersed on nitrogen-doped carbon hollow microspheres (Pt0.38Cu0.62/N-HCS). Benefiting from its structural and compositional advantages, the resulting Pt0.38Cu0.62/N-HCS catalyst delivers exceptional electrocatalytic activity for ORR, with a half-wave potential (E1/2) of 0.837 V, a mass activity of 0.672 A mgPt-1, and a Tafel slope of 50.66 mV dec-1, surpassing that of commercial Pt/C. Moreover, the Pt0.38Cu0.62/N-HCS follows the desired four-electron transfer mechanism throughout the ORR process, thereby displaying a high selectivity for direct reduction of O2 to H2O. Remarkably, this catalyst also showcases high stability, with only a 25 mV drop in E1/2 after 10,000 cycles in an acidic electrolyte. Theoretical calculations elucidate the incorporation of Cu into Pt lattice induces compressive strain, which effectively tailors the d band center of Pt active sites and strengthens the surface chemisorption of O2 molecules on PtCu alloys. Consequently, the Pt0.38Cu0.62/N-HCS catalyst exhibits an improved ability to adsorb O2 molecules on its surface, accelerating the reaction kinetics of O2 conversion to ∗OOH. Additionally, Cu atoms, not only serving as sacrificial anode, undergo preferential oxidation during PEMFCs operation when compared to Pt, but also the stable Cu species in PtCu alloys contributes significantly to maintaining the strain effect, collectively enhancing both activity and durability. Overall, this research offers an effective and promising approach to enhance the activity and stability of Pt-based ORR electrocatalysts in PEMFCs. |
| first_indexed | 2025-02-19T03:36:45Z |
| format | Journal Article |
| id | ntu-10356/178560 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2025-02-19T03:36:45Z |
| publishDate | 2024 |
| record_format | dspace |
| spelling | ntu-10356/1785602024-07-01T15:34:42Z Synergy of compress strain and antioxidant of platinum-copper for enhanced the oxygen reduction performance Zhang, Jun Liang, Pingjuan Xu, Xinlan Wang, Rong Liu, Shuyue Wang, Chunyuan Liu, Boyu Luo, Laizheng Jin, Meng Liu, Huan Yi, Huan Lu, Shi-Yu School of Physical and Mathematical Sciences Engineering Compressive strain Oxygen reduction reaction The development of efficient and durable electrocatalysts for oxygen reduction reaction (ORR) holds a pivotal significance in the successful commercialization of proton exchange membrane fuel cells (PEMFCs) but is still challenging. Herein, we report a worm-liked PtCu nanocrystals dispersed on nitrogen-doped carbon hollow microspheres (Pt0.38Cu0.62/N-HCS). Benefiting from its structural and compositional advantages, the resulting Pt0.38Cu0.62/N-HCS catalyst delivers exceptional electrocatalytic activity for ORR, with a half-wave potential (E1/2) of 0.837 V, a mass activity of 0.672 A mgPt-1, and a Tafel slope of 50.66 mV dec-1, surpassing that of commercial Pt/C. Moreover, the Pt0.38Cu0.62/N-HCS follows the desired four-electron transfer mechanism throughout the ORR process, thereby displaying a high selectivity for direct reduction of O2 to H2O. Remarkably, this catalyst also showcases high stability, with only a 25 mV drop in E1/2 after 10,000 cycles in an acidic electrolyte. Theoretical calculations elucidate the incorporation of Cu into Pt lattice induces compressive strain, which effectively tailors the d band center of Pt active sites and strengthens the surface chemisorption of O2 molecules on PtCu alloys. Consequently, the Pt0.38Cu0.62/N-HCS catalyst exhibits an improved ability to adsorb O2 molecules on its surface, accelerating the reaction kinetics of O2 conversion to ∗OOH. Additionally, Cu atoms, not only serving as sacrificial anode, undergo preferential oxidation during PEMFCs operation when compared to Pt, but also the stable Cu species in PtCu alloys contributes significantly to maintaining the strain effect, collectively enhancing both activity and durability. Overall, this research offers an effective and promising approach to enhance the activity and stability of Pt-based ORR electrocatalysts in PEMFCs. Published version This research was funded by the Young Elite Scientists Sponsorship Program by CAST (2021QNRC001), Natural Science Foundation of Chongqing (CSTB2022NSCQ-MSX0557, cstb2023nscq-msx0979), Talent Introduction of Chongqing University of Science and Technology (ckrc2021050, ckrc20230401, ckrc2021053), the Science and Technology Research Program of Chongqing Municipal Education Commission (KJQN202201532, KJQN202301542), the National Natural Science Foundation of China (22109016) and Open Research Fund of CNMGE Platform & NSCC-TJ (CNMGE2023016). 2024-06-26T02:27:54Z 2024-06-26T02:27:54Z 2024 Journal Article Zhang, J., Liang, P., Xu, X., Wang, R., Liu, S., Wang, C., Liu, B., Luo, L., Jin, M., Liu, H., Yi, H. & Lu, S. (2024). Synergy of compress strain and antioxidant of platinum-copper for enhanced the oxygen reduction performance. Nano Materials Science. https://dx.doi.org/10.1016/j.nanoms.2024.02.011 2589-9651 https://hdl.handle.net/10356/178560 10.1016/j.nanoms.2024.02.011 2-s2.0-85188555766 en Nano Materials Science © 2024 Chongqing University. Publishing services by Elsevier B.V. on behalf of KeAi Communications Co. Ltd. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/). application/pdf |
| spellingShingle | Engineering Compressive strain Oxygen reduction reaction Zhang, Jun Liang, Pingjuan Xu, Xinlan Wang, Rong Liu, Shuyue Wang, Chunyuan Liu, Boyu Luo, Laizheng Jin, Meng Liu, Huan Yi, Huan Lu, Shi-Yu Synergy of compress strain and antioxidant of platinum-copper for enhanced the oxygen reduction performance |
| title | Synergy of compress strain and antioxidant of platinum-copper for enhanced the oxygen reduction performance |
| title_full | Synergy of compress strain and antioxidant of platinum-copper for enhanced the oxygen reduction performance |
| title_fullStr | Synergy of compress strain and antioxidant of platinum-copper for enhanced the oxygen reduction performance |
| title_full_unstemmed | Synergy of compress strain and antioxidant of platinum-copper for enhanced the oxygen reduction performance |
| title_short | Synergy of compress strain and antioxidant of platinum-copper for enhanced the oxygen reduction performance |
| title_sort | synergy of compress strain and antioxidant of platinum copper for enhanced the oxygen reduction performance |
| topic | Engineering Compressive strain Oxygen reduction reaction |
| url | https://hdl.handle.net/10356/178560 |
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