Sr-induced Fermi Engineering of β-FeOOH for Multifunctional Catalysis
© 2024 Wiley-VCH GmbH..
Designing a multifunctional electrocatalyst to produce H2 from water, urea, urine, and wastewater, is highly desirable yet challenging because it demands precise Fermi-engineering to realize stronger π-donation from O 2p to electron(e- )-deficient metal (t2g ) d-orbitals. Here a Sr-induced phase transformed β-FeOOH/α-Ni(OH)2 catalyst anchored on Ni-foam (designated as pt-NFS) is introduced, where Sr produces plenteous Fe4+ (Fe3+ → Fe4+ ) to modulate Fermi level and e- -transfer from e- -rich Ni3+ (t2g )-orbitals to e- -deficient Fe4+ (t2g )-orbitals, via strong π-donation from the π-symmetry lone-pair of O bridge. pt-NFS utilizes Fe-sites near the Sr-atom to break the H─O─H bonds and weakens the adsorption of *O while strengthening that of *OOH, toward hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), respectively. Invaluably, Fe-sites of pt-NFS activate H2 -production from urea oxidation reaction (UOR) through a one-stage pathway which, unlike conventional two-stage pathways with two NH3 -molecules, involves only one NH3 -molecule. Owing to more suitable kinetic energetics, pt-NFS requires 133 mV (negative potential shift), 193 mV, ≈1.352 V, and ≈1.375 V versus RHE for HER, OER, UOR, and human urine oxidation, respectively, to reach the benchmark 10 mA cm-2 and also demonstrates remarkable durability of over 25 h. This work opens a new corridor to design multifunctional electrocatalysts with precise Fermi engineering through d-band modulation.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2024 |
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| Erschienen: |
2024 |
| Enthalten in: |
Zur Gesamtaufnahme - year:2024 |
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| Enthalten in: |
Small methods - (2024) vom: 18. Jan., Seite e2301434 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Ahmad, Waqar [VerfasserIn] |
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| Links: |
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| Themen: |
D-band center |
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| Anmerkungen: |
Date Revised 18.01.2024 published: Print-Electronic Citation Status Publisher |
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| doi: |
10.1002/smtd.202301434 |
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| funding: |
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| Förderinstitution / Projekttitel: |
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| PPN (Katalog-ID): |
NLM367275872 |
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| 520 | |a Designing a multifunctional electrocatalyst to produce H2 from water, urea, urine, and wastewater, is highly desirable yet challenging because it demands precise Fermi-engineering to realize stronger π-donation from O 2p to electron(e- )-deficient metal (t2g ) d-orbitals. Here a Sr-induced phase transformed β-FeOOH/α-Ni(OH)2 catalyst anchored on Ni-foam (designated as pt-NFS) is introduced, where Sr produces plenteous Fe4+ (Fe3+ → Fe4+ ) to modulate Fermi level and e- -transfer from e- -rich Ni3+ (t2g )-orbitals to e- -deficient Fe4+ (t2g )-orbitals, via strong π-donation from the π-symmetry lone-pair of O bridge. pt-NFS utilizes Fe-sites near the Sr-atom to break the H─O─H bonds and weakens the adsorption of *O while strengthening that of *OOH, toward hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), respectively. Invaluably, Fe-sites of pt-NFS activate H2 -production from urea oxidation reaction (UOR) through a one-stage pathway which, unlike conventional two-stage pathways with two NH3 -molecules, involves only one NH3 -molecule. Owing to more suitable kinetic energetics, pt-NFS requires 133 mV (negative potential shift), 193 mV, ≈1.352 V, and ≈1.375 V versus RHE for HER, OER, UOR, and human urine oxidation, respectively, to reach the benchmark 10 mA cm-2 and also demonstrates remarkable durability of over 25 h. This work opens a new corridor to design multifunctional electrocatalysts with precise Fermi engineering through d-band modulation | ||
| 650 | 4 | |a Journal Article | |
| 650 | 4 | |a d-band center | |
| 650 | 4 | |a electronic structure | |
| 650 | 4 | |a fermi engineering | |
| 650 | 4 | |a lattice expansion | |
| 650 | 4 | |a multifunctional catalysis | |
| 650 | 4 | |a phase transform | |
| 700 | 1 | |a Hou, Yunpeng |e verfasserin |4 aut | |
| 700 | 1 | |a Ahmad, Nisar |e verfasserin |4 aut | |
| 700 | 1 | |a Wang, Kun |e verfasserin |4 aut | |
| 700 | 1 | |a Zou, Chenghao |e verfasserin |4 aut | |
| 700 | 1 | |a Wan, Zhengwei |e verfasserin |4 aut | |
| 700 | 1 | |a Aftab, Sumaira |e verfasserin |4 aut | |
| 700 | 1 | |a Zhou, Shaodong |e verfasserin |4 aut | |
| 700 | 1 | |a Pan, Zhao |e verfasserin |4 aut | |
| 700 | 1 | |a Gao, Huai-Ling |e verfasserin |4 aut | |
| 700 | 1 | |a Liang, Chengdu |e verfasserin |4 aut | |
| 700 | 1 | |a Yan, Wenjun |e verfasserin |4 aut | |
| 700 | 1 | |a Ling, Min |e verfasserin |4 aut | |
| 700 | 1 | |a Lu, Zhihui |e verfasserin |4 aut | |
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