ALD-made noble metal high entropy alloy nanofilm with sub-surface amorphization for enhanced hydrogen evolution
Noble metal-based high entropy alloys (NM-HEAs) have been shown to have optimized catalytic properties through compositional adjustments. Recently, an amorphous HEA, known as high-entropy metallic glass (HEMG), has gained attention for its potential in surface modification and atomic rearrangement....
| Main Authors: | , , , , , , , , |
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| Format: | Journal Article |
| Language: | English |
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2024
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| Online Access: | https://hdl.handle.net/10356/178051 |
| _version_ | 1826114528609304576 |
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| author | Zou, Yiming Jing, Lin Zhang, Jianghong Luo, Songzhu Wang, Leyan Li, Yun Goei, Ronn Tan, Kwan Wee Tok, Alfred Iing Yoong |
| author2 | School of Materials Science and Engineering |
| author_facet | School of Materials Science and Engineering Zou, Yiming Jing, Lin Zhang, Jianghong Luo, Songzhu Wang, Leyan Li, Yun Goei, Ronn Tan, Kwan Wee Tok, Alfred Iing Yoong |
| author_sort | Zou, Yiming |
| collection | NTU |
| description | Noble metal-based high entropy alloys (NM-HEAs) have been shown to have optimized catalytic properties through compositional adjustments. Recently, an amorphous HEA, known as high-entropy metallic glass (HEMG), has gained attention for its potential in surface modification and atomic rearrangement. In this work, RhRuPtPdIr HEA thin films (Rh : Ru : Pt : Pd : Ir = 26.1 : 28.7 : 8.6 : 16.3 : 20.3) were synthesized on glassy carbon (GC) electrodes using precisely controlled sequential atomic layer deposition (ALD) process of each noble metal layer, followed by electrical Joule heating (EJH) alloying at 1000 °C for 5 seconds. Cross-sectional HR-TEM imaging revealed a thickness of 20 nm and the surface microstructure composed of nanocrystallites and amorphous structures, suggesting explosive crystallization during the EJH process. The HEA thin film achieved outstanding HER performance, exhibiting overpotentials of 13, 77, and 65 mV at a current density of 10 mA cm−2 and Tafel slopes of 14, 45, and 78 mV dec−1 in 0.5 M H2SO4, 1.0 M PBS, and 1.0 M KOH electrolytes, respectively. Remarkably, HEA/GC in an acidic environment reached strikingly top-level kinetics, which was mainly contributed by intrinsic activity and surface amorphization. The corresponding DFT study revealed a modified electronic structure of the HEA surface that facilitates surface-hydrogen interaction. The study demonstrates the potential of NM-HEA nanofilm as catalysts for highly efficient HER in harsh environments. This study also demonstrates that ALD-EJH is a novel and reliable method for synthesizing, manipulating, and tuning complex high-entropy nanomaterials. |
| first_indexed | 2024-10-01T03:40:36Z |
| format | Journal Article |
| id | ntu-10356/178051 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T03:40:36Z |
| publishDate | 2024 |
| record_format | dspace |
| spelling | ntu-10356/1780512024-06-07T15:44:57Z ALD-made noble metal high entropy alloy nanofilm with sub-surface amorphization for enhanced hydrogen evolution Zou, Yiming Jing, Lin Zhang, Jianghong Luo, Songzhu Wang, Leyan Li, Yun Goei, Ronn Tan, Kwan Wee Tok, Alfred Iing Yoong School of Materials Science and Engineering Engineering Catalytic properties High entropy alloys Noble metal-based high entropy alloys (NM-HEAs) have been shown to have optimized catalytic properties through compositional adjustments. Recently, an amorphous HEA, known as high-entropy metallic glass (HEMG), has gained attention for its potential in surface modification and atomic rearrangement. In this work, RhRuPtPdIr HEA thin films (Rh : Ru : Pt : Pd : Ir = 26.1 : 28.7 : 8.6 : 16.3 : 20.3) were synthesized on glassy carbon (GC) electrodes using precisely controlled sequential atomic layer deposition (ALD) process of each noble metal layer, followed by electrical Joule heating (EJH) alloying at 1000 °C for 5 seconds. Cross-sectional HR-TEM imaging revealed a thickness of 20 nm and the surface microstructure composed of nanocrystallites and amorphous structures, suggesting explosive crystallization during the EJH process. The HEA thin film achieved outstanding HER performance, exhibiting overpotentials of 13, 77, and 65 mV at a current density of 10 mA cm−2 and Tafel slopes of 14, 45, and 78 mV dec−1 in 0.5 M H2SO4, 1.0 M PBS, and 1.0 M KOH electrolytes, respectively. Remarkably, HEA/GC in an acidic environment reached strikingly top-level kinetics, which was mainly contributed by intrinsic activity and surface amorphization. The corresponding DFT study revealed a modified electronic structure of the HEA surface that facilitates surface-hydrogen interaction. The study demonstrates the potential of NM-HEA nanofilm as catalysts for highly efficient HER in harsh environments. This study also demonstrates that ALD-EJH is a novel and reliable method for synthesizing, manipulating, and tuning complex high-entropy nanomaterials. Agency for Science, Technology and Research (A*STAR) Ministry of Education (MOE) Published version This work was supported by the Agency for Science, Technology, and Research (A*STAR) AME Individual Research Grant (IRG) A1983c0032. K. W. T. and L. W. acknowledge financial support from the Singapore Ministry of Education AcRF Tier 2 grant (MOET2EP 50221-0017). 2024-06-04T04:33:05Z 2024-06-04T04:33:05Z 2024 Journal Article Zou, Y., Jing, L., Zhang, J., Luo, S., Wang, L., Li, Y., Goei, R., Tan, K. W. & Tok, A. I. Y. (2024). ALD-made noble metal high entropy alloy nanofilm with sub-surface amorphization for enhanced hydrogen evolution. Journal of Materials Chemistry A, 12(10), 5668-5678. https://dx.doi.org/10.1039/d3ta05908a 2050-7488 https://hdl.handle.net/10356/178051 10.1039/d3ta05908a 2-s2.0-85186263143 10 12 5668 5678 en A1983c0032 MOET2EP 50221-0017 Journal of Materials Chemistry A © The Authors. This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. application/pdf |
| spellingShingle | Engineering Catalytic properties High entropy alloys Zou, Yiming Jing, Lin Zhang, Jianghong Luo, Songzhu Wang, Leyan Li, Yun Goei, Ronn Tan, Kwan Wee Tok, Alfred Iing Yoong ALD-made noble metal high entropy alloy nanofilm with sub-surface amorphization for enhanced hydrogen evolution |
| title | ALD-made noble metal high entropy alloy nanofilm with sub-surface amorphization for enhanced hydrogen evolution |
| title_full | ALD-made noble metal high entropy alloy nanofilm with sub-surface amorphization for enhanced hydrogen evolution |
| title_fullStr | ALD-made noble metal high entropy alloy nanofilm with sub-surface amorphization for enhanced hydrogen evolution |
| title_full_unstemmed | ALD-made noble metal high entropy alloy nanofilm with sub-surface amorphization for enhanced hydrogen evolution |
| title_short | ALD-made noble metal high entropy alloy nanofilm with sub-surface amorphization for enhanced hydrogen evolution |
| title_sort | ald made noble metal high entropy alloy nanofilm with sub surface amorphization for enhanced hydrogen evolution |
| topic | Engineering Catalytic properties High entropy alloys |
| url | https://hdl.handle.net/10356/178051 |
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