Enhancing Nitrate Reduction to Ammonia Through Crystal Phase Engineering : Unveiling the Hydrogen Bonding Effect in δ-FeOOH Electrocatalysis
© 2024 Wiley-VCH GmbH..
Crystal phase engineering has emerged as a powerful tool for tailoring the electrocatalytic performance, yet its impact on nitrate reduction to ammonia (NRA) remains largely uncharted territory. Herein, density functional theory (DFT) calculations are performed to unravel the influence of the crystal phase of FeOOH on the adsorption behavior of *NO3 . Inspiringly, FeOOH samples with four distinct crystal phases (δ, γ, α, and β) are successfully synthesized and deployed as electrocatalysts for NRA. Remarkably, among all FeOOH samples, δ-FeOOH demonstrates the superior NRA performance, achieving a NH3 Faradic efficiency ( FE NH 3 $\rm{FE} _ {\rm{NH_3}}$ ) of 90.2% at -1.0 V versus reversible hydrogen electrode (RHE) and a NH3 yield rate ( Yield NH 3 $\rm{Yield} _ {\rm{NH_3}}$ ) of 5.73 mg h-1 cm-2 at -1.2 V. In-depth experiments and theoretical calculations unveil the existence of hydrogen bonding interaction between δ-FeOOH and *NOx , which not only enhances the adsorption of *NOx but also disrupts the linear relationships between the free energy of *NO3 adsorption and various parameters, including limiting potential, d-band center (εd ) and transferred charge from FeOOH to *NO3 , ultimately contributing to the exceptional NRA performance.
| 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 (Weinheim an der Bergstrasse, Germany) - (2024) vom: 01. März, Seite e2401327 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Qu, Kaiyu [VerfasserIn] |
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| Links: |
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| Themen: |
Breaking linear scaling relationships |
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| Anmerkungen: |
Date Revised 01.03.2024 published: Print-Electronic Citation Status Publisher |
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| doi: |
10.1002/smll.202401327 |
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| funding: |
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| Förderinstitution / Projekttitel: |
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| PPN (Katalog-ID): |
NLM369191498 |
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| 100 | 1 | |a Qu, Kaiyu |e verfasserin |4 aut | |
| 245 | 1 | 0 | |a Enhancing Nitrate Reduction to Ammonia Through Crystal Phase Engineering |b Unveiling the Hydrogen Bonding Effect in δ-FeOOH Electrocatalysis |
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| 500 | |a Date Revised 01.03.2024 | ||
| 500 | |a published: Print-Electronic | ||
| 500 | |a Citation Status Publisher | ||
| 520 | |a © 2024 Wiley-VCH GmbH. | ||
| 520 | |a Crystal phase engineering has emerged as a powerful tool for tailoring the electrocatalytic performance, yet its impact on nitrate reduction to ammonia (NRA) remains largely uncharted territory. Herein, density functional theory (DFT) calculations are performed to unravel the influence of the crystal phase of FeOOH on the adsorption behavior of *NO3 . Inspiringly, FeOOH samples with four distinct crystal phases (δ, γ, α, and β) are successfully synthesized and deployed as electrocatalysts for NRA. Remarkably, among all FeOOH samples, δ-FeOOH demonstrates the superior NRA performance, achieving a NH3 Faradic efficiency ( FE NH 3 $\rm{FE} _ {\rm{NH_3}}$ ) of 90.2% at -1.0 V versus reversible hydrogen electrode (RHE) and a NH3 yield rate ( Yield NH 3 $\rm{Yield} _ {\rm{NH_3}}$ ) of 5.73 mg h-1 cm-2 at -1.2 V. In-depth experiments and theoretical calculations unveil the existence of hydrogen bonding interaction between δ-FeOOH and *NOx , which not only enhances the adsorption of *NOx but also disrupts the linear relationships between the free energy of *NO3 adsorption and various parameters, including limiting potential, d-band center (εd ) and transferred charge from FeOOH to *NO3 , ultimately contributing to the exceptional NRA performance | ||
| 650 | 4 | |a Journal Article | |
| 650 | 4 | |a breaking linear scaling relationships | |
| 650 | 4 | |a crystal phase engineering | |
| 650 | 4 | |a hydrogen bonds | |
| 650 | 4 | |a nitrate reduction reactions | |
| 700 | 1 | |a Zhu, Xiaojuan |e verfasserin |4 aut | |
| 700 | 1 | |a Zhang, Yu |e verfasserin |4 aut | |
| 700 | 1 | |a Song, Leyang |e verfasserin |4 aut | |
| 700 | 1 | |a Wang, Jing |e verfasserin |4 aut | |
| 700 | 1 | |a Gong, Yushuang |e verfasserin |4 aut | |
| 700 | 1 | |a Liu, Xiang |e verfasserin |4 aut | |
| 700 | 1 | |a Wang, An-Liang |e verfasserin |4 aut | |
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| 773 | 1 | 8 | |g year:2024 |g day:01 |g month:03 |g pages:e2401327 |
| 856 | 4 | 0 | |u http://dx.doi.org/10.1002/smll.202401327 |3 Volltext |
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