Abstract:The S-NiFeV LDH catalyst exhibits exceptional catalytic activity and stability toward the urea oxidation reaction via a sulfur-doping strategy.
“…The potential for NiCo 2 S 4 @NiMn LDH at a current density of 100 mA·cm –2 fell by 211 mV compared to the catalytic activity in 1.0 M KOH at the same current density, illustrating its excellent UOR performance. Furthermore, a response is observed for NiCo 2 S 4 @NiMn LDH in the absence of urea, deriving from the oxidation of the Ni 2+ species . To investigate the UOR reaction kinetics of the catalysts in more detail, Tafel slopes were derived from the corresponding polarization curves (Figure d).…”
Section: Resultsmentioning
confidence: 99%
“…Furthermore, a response is observed for NiCo 2 S 4 @NiMn LDH in the absence of urea, deriving from the oxidation of the Ni 2+ species. 56 To investigate the UOR reaction kinetics of the catalysts in more detail, Tafel slopes were derived from the corresponding polarization curves (Figure 4d). NiCo 2 S 4 @NiMn LDH exhibited a very low Tafel slope of 43.8 mV•dec −1 , which was much lower than that of NiCo 2 S 4 (69.2 mV•dec −1 ), NiMn LDH (95.9 mV•dec −1 ), and commercial RuO 2 (118.1 mV•dec −1 ), indicating an accelerated UOR kinetics process due to the formation of a heterogeneous interface and synergistic effects between the NiCo 2 S 4 and NiMn LDH.…”
Section: Resultsmentioning
confidence: 99%
“…In line with the LSV curves, the lowest charge transfer resistance (R ct ) for the NiCo 2 S 4 @NiMn LDH catalyst was 1.34 Ω, lower than that of NiCo 2 S 4 (1.37 Ω), NiMn LDH (1.41 Ω), commercial RuO 2 (1.79 Ω), and NF (3.96 Ω), illustrating the enhanced electron transfer efficiency at the electrode−electrolyte interface and advanced UOR kinetics of the unique heterostructure in comparison with its individual counterparts. 18,56 The ECSA is an important parameter for the estimation of the activity of a catalyst. In the present study, it was calculated based on the electrochemical C dl obtained from the CV curves produced at various scan rates in the non-Faradaic potential region (Figure S5).…”
Section: Resultsmentioning
confidence: 99%
“…NiCo 2 S 4 @NiMn LDH exhibited a very low Tafel slope of 43.8 mV·dec –1 , which was much lower than that of NiCo 2 S 4 (69.2 mV·dec –1 ), NiMn LDH (95.9 mV·dec –1 ), and commercial RuO 2 (118.1 mV·dec –1 ), indicating an accelerated UOR kinetics process due to the formation of a heterogeneous interface and synergistic effects between the NiCo 2 S 4 and NiMn LDH. , EIS tests were also conducted to investigate the UOR kinetics and electrode–electrolyte interface behavior with the fitted Nyquist plots for the samples presented in Figure e. In line with the LSV curves, the lowest charge transfer resistance ( R ct ) for the NiCo 2 S 4 @NiMn LDH catalyst was 1.34 Ω, lower than that of NiCo 2 S 4 (1.37 Ω), NiMn LDH (1.41 Ω), commercial RuO 2 (1.79 Ω), and NF (3.96 Ω), illustrating the enhanced electron transfer efficiency at the electrode–electrolyte interface and advanced UOR kinetics of the unique heterostructure in comparison with its individual counterparts. , …”
The rational design of advanced transition-metal-based
electrocatalysts
with a heterostructure is a promising strategy for the promotion of
the urea oxidation reaction (UOR) for energy-conservation technologies,
but achieving a sufficiently high performance remains a challenge.
In this work, we report a dramatic improvement in the UOR performance
of a heterostructured electrocatalyst that combines NiMn-layered double
hydroxide (LDH) nanosheets with NiCo2S4 arrays
via a series of facile hydrothermal fabrication steps. Due to the
high-flux electron transfer pathways at the close-contact interface,
abundant active sites, and unique three-dimensional (3D) architecture,
the NiCo2S4@NiMn LDH heterostructure grown on
nickel foam exhibits a low potential of 1.37 V at a current density
of 100 mA·cm–2 and a low Tafel slope of 43.8
mV·dec–1. More impressively, the proposed electrocatalyst
demonstrates robust stability of more than 25 h at a current density
of 50 mA·cm–2 with a negligible decrease in
activity. In addition, density functional theory calculations reveal
that the interface engineering within the heterostructure is beneficial
for the adsorption and activation of urea molecules and the improvement
of the sluggish UOR dynamics. The dissociation of adsorbed CO(NH2)2* into CO* and NH* intermediates on the heterostructured
NiMn LDH is also facilitated by electronic coupling with NiCo2S4, resulting in superior UOR performance.
“…The potential for NiCo 2 S 4 @NiMn LDH at a current density of 100 mA·cm –2 fell by 211 mV compared to the catalytic activity in 1.0 M KOH at the same current density, illustrating its excellent UOR performance. Furthermore, a response is observed for NiCo 2 S 4 @NiMn LDH in the absence of urea, deriving from the oxidation of the Ni 2+ species . To investigate the UOR reaction kinetics of the catalysts in more detail, Tafel slopes were derived from the corresponding polarization curves (Figure d).…”
Section: Resultsmentioning
confidence: 99%
“…Furthermore, a response is observed for NiCo 2 S 4 @NiMn LDH in the absence of urea, deriving from the oxidation of the Ni 2+ species. 56 To investigate the UOR reaction kinetics of the catalysts in more detail, Tafel slopes were derived from the corresponding polarization curves (Figure 4d). NiCo 2 S 4 @NiMn LDH exhibited a very low Tafel slope of 43.8 mV•dec −1 , which was much lower than that of NiCo 2 S 4 (69.2 mV•dec −1 ), NiMn LDH (95.9 mV•dec −1 ), and commercial RuO 2 (118.1 mV•dec −1 ), indicating an accelerated UOR kinetics process due to the formation of a heterogeneous interface and synergistic effects between the NiCo 2 S 4 and NiMn LDH.…”
Section: Resultsmentioning
confidence: 99%
“…In line with the LSV curves, the lowest charge transfer resistance (R ct ) for the NiCo 2 S 4 @NiMn LDH catalyst was 1.34 Ω, lower than that of NiCo 2 S 4 (1.37 Ω), NiMn LDH (1.41 Ω), commercial RuO 2 (1.79 Ω), and NF (3.96 Ω), illustrating the enhanced electron transfer efficiency at the electrode−electrolyte interface and advanced UOR kinetics of the unique heterostructure in comparison with its individual counterparts. 18,56 The ECSA is an important parameter for the estimation of the activity of a catalyst. In the present study, it was calculated based on the electrochemical C dl obtained from the CV curves produced at various scan rates in the non-Faradaic potential region (Figure S5).…”
Section: Resultsmentioning
confidence: 99%
“…NiCo 2 S 4 @NiMn LDH exhibited a very low Tafel slope of 43.8 mV·dec –1 , which was much lower than that of NiCo 2 S 4 (69.2 mV·dec –1 ), NiMn LDH (95.9 mV·dec –1 ), and commercial RuO 2 (118.1 mV·dec –1 ), indicating an accelerated UOR kinetics process due to the formation of a heterogeneous interface and synergistic effects between the NiCo 2 S 4 and NiMn LDH. , EIS tests were also conducted to investigate the UOR kinetics and electrode–electrolyte interface behavior with the fitted Nyquist plots for the samples presented in Figure e. In line with the LSV curves, the lowest charge transfer resistance ( R ct ) for the NiCo 2 S 4 @NiMn LDH catalyst was 1.34 Ω, lower than that of NiCo 2 S 4 (1.37 Ω), NiMn LDH (1.41 Ω), commercial RuO 2 (1.79 Ω), and NF (3.96 Ω), illustrating the enhanced electron transfer efficiency at the electrode–electrolyte interface and advanced UOR kinetics of the unique heterostructure in comparison with its individual counterparts. , …”
The rational design of advanced transition-metal-based
electrocatalysts
with a heterostructure is a promising strategy for the promotion of
the urea oxidation reaction (UOR) for energy-conservation technologies,
but achieving a sufficiently high performance remains a challenge.
In this work, we report a dramatic improvement in the UOR performance
of a heterostructured electrocatalyst that combines NiMn-layered double
hydroxide (LDH) nanosheets with NiCo2S4 arrays
via a series of facile hydrothermal fabrication steps. Due to the
high-flux electron transfer pathways at the close-contact interface,
abundant active sites, and unique three-dimensional (3D) architecture,
the NiCo2S4@NiMn LDH heterostructure grown on
nickel foam exhibits a low potential of 1.37 V at a current density
of 100 mA·cm–2 and a low Tafel slope of 43.8
mV·dec–1. More impressively, the proposed electrocatalyst
demonstrates robust stability of more than 25 h at a current density
of 50 mA·cm–2 with a negligible decrease in
activity. In addition, density functional theory calculations reveal
that the interface engineering within the heterostructure is beneficial
for the adsorption and activation of urea molecules and the improvement
of the sluggish UOR dynamics. The dissociation of adsorbed CO(NH2)2* into CO* and NH* intermediates on the heterostructured
NiMn LDH is also facilitated by electronic coupling with NiCo2S4, resulting in superior UOR performance.
“…2f, it can be divided into two distinct components, where the characteristic peaks at 530.88 eV and 531.98 eV are attributed to O-H bonds and surface-adsorbed oxygen, respectively. 28 The morphology of the prepared catalysts is also characterized by SEM and TEM. As shown by SEM in Fig.…”
The rational modification of electronic structures for catalytic active sites has been proved to be a promising strategy to facilitate efficient urea oxidation reaction (UOR). Herein, in this work, a...
The development of highly efficient urea oxidation reaction (UOR) electrocatalysts is the key to simultaneously achieving green hydrogen production and the treatment of urea‐containing wastewater. Ni‐based electrocatalysts are expected to replace precious metal catalysts for UOR because of their high activity and low cost. However, the construction of Ni‐based electrocatalysts that can synergistically enhance UOR still needs further in‐depth study. In this study, highly active electrocatalysts of NiFe(OH)x/MnO2 p‐p heterostructures are constructed on nickel foam (NF) by electrodeposition (NiFe(OH)x/MnO2/NF), illustrating the effect of electronic structure changes at heterogeneous interfaces on UOR and revealing the catalytic mechanism of UOR. The NiFe(OH)x/MnO2/NF only needs 1.364 V (vs Reversible Hydrogen Electrode, RHE) to reach 10 mA cm−2 for UOR. Structural characterizations and theoretical calculations indicate that energy gap leads to directed charge transfer and redistribution at the heterojunction interface, forming electron‐rich (MnO2) and electron‐poor (NiFe(OH)x) regions. This enhances the catalyst's adsorption of urea and reaction intermediates, reduces thermodynamic barriers during the UOR process, promotes the formation of Ni3+ phases at lower potentials, and thus improves UOR performance. This work provides a new idea for the development of Ni‐based high‐efficiency UOR electrocatalysts.
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