A general but still unknown characteristic of active oxygen evolution electrocatalysts

Illas, Francesc; Calle‐Vallejo, Federico; Romeo, Eleonora

doi:10.1039/d2sc06832j

Cited by 17 publications

(11 citation statements)

References 43 publications

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“…This observation agrees with the rate-determining step (RDS) of experimental observations as well . It is worth noting that even though there is a conceptual difference between the PLS and the RDS, they are often connected in multistep electrocatalytic reaction pathways. − Hence, in this analysis, it was presumed to correspond. Further work maybe required for confirmation.…”

Section: Resultssupporting

confidence: 82%

MXenes as Effective Sulfur Hosts and Electrocatalysts to Suppress Lithium Polysulfide Shuttling: A Computational Study

Boteju,

Ponnurangam,

Thangadurai

2024

J. Phys. Chem. C

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Exploring electrocatalysts for the sulfur reduction reaction (SRR) has emerged as a promising strategy to suppress the shuttle effect and enhance the kinetics in lithium−sulfur (Li−S) batteries. A comprehensive understanding of the electrocatalytic mechanism within Li−S batteries remains elusive, which hinders the rational design of advanced electrocatalysts for these systems. In this study, two-dimensional (2D) transition metal carbides and nitrides (MXenes) have been investigated for the catalytic conversion of lithium polysulfides (LiPSs) using density functional theory (DFT). Our findings reveal that MXenes show a moderate binding affinity for LiPSs, suggesting favorable thermodynamics for their role as electrocatalysts for the SRR. This thermodynamic favorability promotes the suppression of the LiPSs' shuttle effect and the enhancement of the SRR kinetics. The SRR process in Li−S batteries consists of multiple steps with varying activation energies. Our analysis by constructing the energy diagram for the multistep SRR indicates that the initial reduction of S 8 to Li 2 S 8 is facile with a lower activation energy, while the last step where Li 2 S 2 converts to Li 2 S appears to be a rate-limiting step. To predict the catalytic abilities of MXene structures, we built a volcano-shaped relationship between the adsorption of LiPSs and catalytic activity. We show three MXenes�Ta 2 CO 2 , Zr 2 NO 2 , and Mo 2 NO 2 as potential electrocatalysts that exhibit lower thermodynamic overpotentials for the SRR. These findings represent a significant step toward developing advanced electrocatalysts that may unlock the full potential of Li−S batteries, paving the way for improved energy storage systems with enhanced efficiency and performance.

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Section: Resultssupporting

confidence: 82%

MXenes as Effective Sulfur Hosts and Electrocatalysts to Suppress Lithium Polysulfide Shuttling: A Computational Study

Boteju,

Ponnurangam,

Thangadurai

2024

J. Phys. Chem. C

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“…The ε d of Fe 3d shifts to low energy level with the decrease of Fe coordination number (Figure b,e), implying the changes of adsorption behavior for *OOH, *O, and *OH. The electrochemical symmetry of CoFe 2 O 4 and CoFe 2 O 4 –C d was then evaluated by estimating the electrochemical-step symmetry index (ESSI), which is close to zero for the ideal catalysts Figure c,f are the OER free energy diagram for CoFe 2 O 4 (100) and CoFe 2 O 4 –C d (100).…”

Section: Results and Discussionmentioning

confidence: 99%

Lowering the Coordination of Octahedra in Spinel Oxides by the Robust Fe–N Bonds for Enhancing Oxygen Evolution Reaction

Wang,

Jia,

Zhao

et al. 2024

ACS Catal.

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The coordination environment of octahedra in spinel oxides plays a vital role in regulating the OER performance. But selectively engineering the octahedral units is very challenging for the design of low-cost and high-efficient electrocatalysts. In this work, the low Fe coordinated CoFe 2 O 4 (CoFe 2 O 4 −C d ) is successfully obtained by taking advantage of the different bond strength between metal centers and N atoms in 7,7,8,8-tetracyanoquinodimethane-decorated CoFe-MOF-74 (CoFe-MOF-74/TCNQ) and shows promising physical and chemical properties. DFT calculations reveal that the low-coordinated Fe improves the electrochemical symmetry of catalysts and reduces the free energy barrier of the potential-determining step, resulting in the high activity and stability of CoFe 2 O 4 −C d . Systematic experimental and theoretical analyses demonstrate that TCNQ motivates the more electron-occupied states at the Fermi level of CoFe-MOF-74 and enhances the hybridization of Co 3d, Fe 3d, and N 2p, leading to the formation of the Co/Fe−N bond. Owing to the stronger Fe−N bonds, CoFe-MOF-74/TCNQ realizes the step-by-step phase transformation upon electrochemical activation, achieving the CoFe 2 O 4 −C d . This work advances the current comprehension of the controllable regulation of coordination environment of octahedra in spinel oxides, which in turn contributes to the design of high-performance electrocatalysts for OER.

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“…67,[79][80][81][82][83][84] Recently, the electrocatalysts design and optimization based on theoretical calculation advanced by leaps and bounds, which has decreased the time cost compared with the ''trial and error'' approach. [85][86][87][88][89][90][91][92] Such development helps us narrows the scope of potential electrocatalyst candidates, pushing the realization of the electrocatalytic NW recycling. However, electrocatalysts have not yet been customized for practical application because of the following technical challenges: (1) the timeand voltage-dependent stability of faradaic efficiency when directly coupled with renewable energy systems; and (2) the lowcost mass preparation of catalysts.…”

Section: Strengthening the Nitrogen Recycling Chain: Design And Macro...mentioning

confidence: 99%

Electrocatalysis of nitrogen pollution: transforming nitrogen waste into high-value chemicals

Wu,

Zhu,

Wallace

et al. 2024

Chem. Soc. Rev.

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A general but still unknown characteristic of active oxygen evolution electrocatalysts

Abstract: The unsatisfactory electrocatalysis of the oxygen evolution reaction (OER) is a major hurdle for the sustainable production of hydrogen using water electrolyzers. Besides, most state-of-the-art catalysts are based on expensive...

Cited by 17 publications

References 43 publications

MXenes as Effective Sulfur Hosts and Electrocatalysts to Suppress Lithium Polysulfide Shuttling: A Computational Study

MXenes as Effective Sulfur Hosts and Electrocatalysts to Suppress Lithium Polysulfide Shuttling: A Computational Study

Lowering the Coordination of Octahedra in Spinel Oxides by the Robust Fe–N Bonds for Enhancing Oxygen Evolution Reaction

Electrocatalysis of nitrogen pollution: transforming nitrogen waste into high-value chemicals

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