Atomically Tailored Zn-ZIF-8 via RuNi Nanoalloy Replacement for Improved Photocatalytic H2 Evolution
In this study, we developed a solid-state atomic replacement method for metal catalysts, enabling the exchange of metal atoms between single atoms and nanoalloys to create new combinations of nanoalloys and single atoms. We observed that partial metal interchange occurred between the RuNi nanoalloy...
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my.uniten.dspace-362702025-03-03T15:41:45Z Atomically Tailored Zn-ZIF-8 via RuNi Nanoalloy Replacement for Improved Photocatalytic H2 Evolution Jamma A. Vennapoosa C.S. Annadata H.V. Ghosh B. Govu R. Aggarwal H. Ahmadipour M. Abraham B.M. Wang X. Pal U. 58136696100 57566914300 56523349500 7202485801 57211414811 37111814400 55533484700 59339085600 57192623231 8908351700 Bioremediation Catalytic cracking Energy conservation Extended X ray absorption fine structure spectroscopy Nanocrystals Photocatalytic activity Sustainable development X ray absorption near edge structure spectroscopy Zero-carbon Zinc alloys Zinc sulfide carbon hydrogen metal alloy nanoparticle nanocrystal nanoparticle nickel nitrogen proton Atomic levels Atomic-level engineering Density functional theory Density-functional-theory Extended X-ray absorption fine structures Hydrogen-evolution Nano-alloys Ni single atom Proton reduction Single-atoms absorption adsorption article atom catalyst controlled study density functional theory electron energy conversion extended X ray absorption fine structure spectroscopy high temperature hydrogen evolution hydrogen evolution reaction pharmaceutics pyrolysis solid state X ray absorption near edge structure spectroscopy X ray analysis Hydrogen evolution reaction In this study, we developed a solid-state atomic replacement method for metal catalysts, enabling the exchange of metal atoms between single atoms and nanoalloys to create new combinations of nanoalloys and single atoms. We observed that partial metal interchange occurred between the RuNi nanoalloy and Zn from the zeolitic imidazolate framework-8 (ZIF-8) on a carbon-nitrogen framework (CNF) at a high temperature of 900 �C, leading to the creation of RuZn nanoparticles and single nickel atoms (Ni-CN). Extended X-ray absorption fine structure (EXAFS) and X-ray absorption near edge structure (XANES) analyses revealed that Ni is atomically dispersed within (RuZn)/Ni-CN. This finding confirms the migration of Zn and Ni during the pyrolysis of the RuNi@ZIF-8 precursor, providing definitive evidence of atomic replacement. Due to the synergistic influence of RuZn nanocrystals and Ni-CN, the resulting (RuZn)/Ni-CN multisite catalyst exhibited superior hydrogen evolution reaction (HER) ability compared to the conventional nanoalloy-based catalysts. Density functional theory calculations revealed that the integration of the (RuZn)n cluster on Ni surrounded with different N-coordinated carbon structures enhanced HER activity with the optimized (RuZn)n/NiN2C2 catalyst exhibiting a low ?GH and improved electron charge redistribution, thereby promoting favorable hydrogen adsorption. Our findings provide valuable insights into the design and optimization of photocatalysts through atomic-level engineering, opening new avenues for efficient and sustainable energy conversion technologies. ? 2024 American Chemical Society. Final 2025-03-03T07:41:45Z 2025-03-03T07:41:45Z 2024 Article 10.1021/acsami.4c11732 2-s2.0-85209578293 https://www.scopus.com/inward/record.uri?eid=2-s2.0-85209578293&doi=10.1021%2facsami.4c11732&partnerID=40&md5=df4c64be178acaebdca96c9fad3cd385 https://irepository.uniten.edu.my/handle/123456789/36270 16 47 64681 64690 American Chemical Society Scopus |
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Bioremediation Catalytic cracking Energy conservation Extended X ray absorption fine structure spectroscopy Nanocrystals Photocatalytic activity Sustainable development X ray absorption near edge structure spectroscopy Zero-carbon Zinc alloys Zinc sulfide carbon hydrogen metal alloy nanoparticle nanocrystal nanoparticle nickel nitrogen proton Atomic levels Atomic-level engineering Density functional theory Density-functional-theory Extended X-ray absorption fine structures Hydrogen-evolution Nano-alloys Ni single atom Proton reduction Single-atoms absorption adsorption article atom catalyst controlled study density functional theory electron energy conversion extended X ray absorption fine structure spectroscopy high temperature hydrogen evolution hydrogen evolution reaction pharmaceutics pyrolysis solid state X ray absorption near edge structure spectroscopy X ray analysis Hydrogen evolution reaction |
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Bioremediation Catalytic cracking Energy conservation Extended X ray absorption fine structure spectroscopy Nanocrystals Photocatalytic activity Sustainable development X ray absorption near edge structure spectroscopy Zero-carbon Zinc alloys Zinc sulfide carbon hydrogen metal alloy nanoparticle nanocrystal nanoparticle nickel nitrogen proton Atomic levels Atomic-level engineering Density functional theory Density-functional-theory Extended X-ray absorption fine structures Hydrogen-evolution Nano-alloys Ni single atom Proton reduction Single-atoms absorption adsorption article atom catalyst controlled study density functional theory electron energy conversion extended X ray absorption fine structure spectroscopy high temperature hydrogen evolution hydrogen evolution reaction pharmaceutics pyrolysis solid state X ray absorption near edge structure spectroscopy X ray analysis Hydrogen evolution reaction Jamma A. Vennapoosa C.S. Annadata H.V. Ghosh B. Govu R. Aggarwal H. Ahmadipour M. Abraham B.M. Wang X. Pal U. Atomically Tailored Zn-ZIF-8 via RuNi Nanoalloy Replacement for Improved Photocatalytic H2 Evolution |
| description |
In this study, we developed a solid-state atomic replacement method for metal catalysts, enabling the exchange of metal atoms between single atoms and nanoalloys to create new combinations of nanoalloys and single atoms. We observed that partial metal interchange occurred between the RuNi nanoalloy and Zn from the zeolitic imidazolate framework-8 (ZIF-8) on a carbon-nitrogen framework (CNF) at a high temperature of 900 �C, leading to the creation of RuZn nanoparticles and single nickel atoms (Ni-CN). Extended X-ray absorption fine structure (EXAFS) and X-ray absorption near edge structure (XANES) analyses revealed that Ni is atomically dispersed within (RuZn)/Ni-CN. This finding confirms the migration of Zn and Ni during the pyrolysis of the RuNi@ZIF-8 precursor, providing definitive evidence of atomic replacement. Due to the synergistic influence of RuZn nanocrystals and Ni-CN, the resulting (RuZn)/Ni-CN multisite catalyst exhibited superior hydrogen evolution reaction (HER) ability compared to the conventional nanoalloy-based catalysts. Density functional theory calculations revealed that the integration of the (RuZn)n cluster on Ni surrounded with different N-coordinated carbon structures enhanced HER activity with the optimized (RuZn)n/NiN2C2 catalyst exhibiting a low ?GH and improved electron charge redistribution, thereby promoting favorable hydrogen adsorption. Our findings provide valuable insights into the design and optimization of photocatalysts through atomic-level engineering, opening new avenues for efficient and sustainable energy conversion technologies. ? 2024 American Chemical Society. |
| author2 |
58136696100 |
| author_facet |
58136696100 Jamma A. Vennapoosa C.S. Annadata H.V. Ghosh B. Govu R. Aggarwal H. Ahmadipour M. Abraham B.M. Wang X. Pal U. |
| format |
Article |
| author |
Jamma A. Vennapoosa C.S. Annadata H.V. Ghosh B. Govu R. Aggarwal H. Ahmadipour M. Abraham B.M. Wang X. Pal U. |
| author_sort |
Jamma A. |
| title |
Atomically Tailored Zn-ZIF-8 via RuNi Nanoalloy Replacement for Improved Photocatalytic H2 Evolution |
| title_short |
Atomically Tailored Zn-ZIF-8 via RuNi Nanoalloy Replacement for Improved Photocatalytic H2 Evolution |
| title_full |
Atomically Tailored Zn-ZIF-8 via RuNi Nanoalloy Replacement for Improved Photocatalytic H2 Evolution |
| title_fullStr |
Atomically Tailored Zn-ZIF-8 via RuNi Nanoalloy Replacement for Improved Photocatalytic H2 Evolution |
| title_full_unstemmed |
Atomically Tailored Zn-ZIF-8 via RuNi Nanoalloy Replacement for Improved Photocatalytic H2 Evolution |
| title_sort |
atomically tailored zn-zif-8 via runi nanoalloy replacement for improved photocatalytic h2 evolution |
| publisher |
American Chemical Society |
| publishDate |
2025 |
| _version_ |
1825816140616564736 |
| score |
13.244413 |