Theoretical inspection of TM-P4C single-atom electrocatalysts: High performance for oxygen reduction and evolution reactions

Guan, Chaohong; Ouyang, Runxin; Zhu, Hong; Xie, Yangyang

doi:10.1016/j.electacta.2022.140853

Cited by 7 publications

(3 citation statements)

References 58 publications

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“…7e and f, it can be found that the total energies of the two systems maintain a very small fluctuation, and even at this high temperature, the structures of the two catalysts have no significant distortion after 2 ps simulations, indicating that the atoms vibrate at the lattice sites to maintain the structure. 46 The analysis mentioned above proves that Rh@g-C 10 N 3 and Ir@g-C 10 N 3 possess excellent stability.…”

Section: Solvation Effect and Further Test Of Stabilitymentioning

confidence: 81%

Theoretical prediction of emerging high-performance trifunctional ORR/OER/HER single-atom catalysts: transition metals anchored into π–π conjugated graphitic carbon nitride (g-C₁₀N₃)

Zhu,

Feng,

Zheng

et al. 2023

Phys. Chem. Chem. Phys.

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Section: Solvation Effect and Further Test Of Stabilitymentioning

confidence: 81%

Theoretical prediction of emerging high-performance trifunctional ORR/OER/HER single-atom catalysts: transition metals anchored into π–π conjugated graphitic carbon nitride (g-C₁₀N₃)

Zhu,

Feng,

Zheng

et al. 2023

Phys. Chem. Chem. Phys.

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“…It is found that the ε d of the Rh atom in the Rh N @C 54 N 71 systems (Figure S15i,j) and Pd atom in the Pd int @C 54 N 72 systems (Figure S16f,g) are moderate. For the bifunctional OER/ORR process, a suitable ε d position (a modest adsorption strengthen of intermediates) plays a key role in screening electrocatalysts, 60 which explains excellent electrocatalytic activities of the Rh N @C 54 N 71 and Pd int @C 54 N 72 systems. In addition, ε d is plotted against ΔG *OH , ΔG *O, and ΔG *OOH in Figure S17.…”

Section: Oer Electrocatalytic Performancementioning

confidence: 99%

Theoretical Insights on the Charge State and Bifunctional OER/ORR Electrocatalyst Activity in 4d-Transition-Metal-Doped g-C₃N₄ Monolayers

Li,

Zhang,

Feng

et al. 2024

ACS Appl. Mater. Interfaces

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Exploring efficient and stable electrocatalysts for the bifunctional oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) is vital to developing renewable energy technologies. However, due to the substantial and intricate design space associated with these bifunctional OER/ORR electrocatalysts, their development presents a formidable challenge, resulting in their cost-prohibitive nature in both experimental and computational studies. Herein, using the defect physics method, we systematically investigate the formation energies and bifunctional overpotential (η Bi ) of 4d-transition-metal (4d-TM, 4d-TM = Zr, Nb, Mo, Ru, Rh, Pd, and Ag)-doped monolayer supercell g-C 3 N 4 (4d-TM@C 54 N 72 ) based on the density functional theory (DFT) calculations. Under N-rich and Crich conditions, we find that the formation energies of Rh N @C 54 N 71 (Rh occupation N) and Pd N @C 54 N 71 (Pd occupation N) are smaller than that of other 4d-TM N @C 54 N 71 (4d-TM occupation N site); for the 4d-TM int @C 54 N 72 (4d-TM interstitial site occupation), the lowest-formation energy defects are Pd int @C 54 N 72 . These results indicate that they have better stabilities. Interestingly, for these formation energy lower systems, Pd 0 int @C 54 N 72 (η Bi = 1.00 V) and Rh 1+ N @C 54 N 71 (η Bi = 0.73 V) have ultralow overpotential and can be great candidates for bifunctional OER/ORR electrocatalysts. We find the reason is that adjusting the charge states of 4d-TM@C 54 N 72 can tune the interaction strength between the oxygenated intermediates and the 4d-TM@ C 54 N 72 , which plays a crucial role in the activity of reactions. Additionally, the data obtained through machine learning (ML) application suggest that the electronegativity (N m ) and bond length of 4d-TM and coordination atoms (d TM-OOH ) are primary descriptors characterizing the OER and ORR activities, respectively. The charged defect tuning of the bifunctional OER/ORR activity for 4d-TM@C 54 N 72 would enable electrocatalytic performance optimization and the development of potential electrocatalysts for renewable energy applications.

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“…When designing a bifunctional catalyst for OER/ORR, Guan and co‐authors anchored transition metal single atoms onto tetra‐coordinated phosphorus‐modified graphene (TMP4). [ 114 ] There is a positive correlation between the bifunctional catalytic activity and the work function, with larger work functions leading to improved bifunctional catalytic performance. The optimal CoP4 catalyst takes advantage of the hybridization between Co‐ d and p orbitals of O‐containing groups, possessing the best OER/ORR bifunctional activity.…”

Section: Work Function‐regulated Material‐electrolyte Iet For Monolit...mentioning

confidence: 99%

Work Function‐Guided Electrocatalyst Design

Chen,

Ma,

Wei

et al. 2024

Advanced Materials

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The development of high‐performance electrocatalysts for energy conversion reactions is crucial for advancing global energy sustainability. The design of catalysts based on their electronic properties (e.g., work function) has gained significant attention recently. Although numerous reviews on electrocatalysis have been provided, no such reports on work function‐guided electrocatalyst design are available. Herein, we provide a comprehensive summary of the latest advancements in work function‐guided electrocatalyst design for diverse electrochemical energy applications. This includes the development of work function‐based catalytic activity descriptors, and the design of both monolithic and heterostructural catalysts. The measurement of work function is first discussed and the applications of work function‐based catalytic activity descriptors for various reactions are fully analyzed. Subsequently, the work function‐regulated material‐electrolyte interfacial electron transfer (IET) is employed for monolithic catalyst design and methods for regulating the work function and optimizing the catalytic performance of catalysts are discussed. In addition, key strategies for tuning the work function‐governed material‐material IET in heterostructural catalyst design are examined. Finally, perspectives on work function determination, work function‐based activity descriptors, and catalyst design are put forward to guide future research. This work paves the way to the work function‐guided rational design of efficient electrocatalysts for sustainable energy applications.This article is protected by copyright. All rights reserved

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Theoretical inspection of TM-P4C single-atom electrocatalysts: High performance for oxygen reduction and evolution reactions

Cited by 7 publications

References 58 publications

Theoretical prediction of emerging high-performance trifunctional ORR/OER/HER single-atom catalysts: transition metals anchored into π–π conjugated graphitic carbon nitride (g-C₁₀N₃)

Theoretical prediction of emerging high-performance trifunctional ORR/OER/HER single-atom catalysts: transition metals anchored into π–π conjugated graphitic carbon nitride (g-C₁₀N₃)

Theoretical Insights on the Charge State and Bifunctional OER/ORR Electrocatalyst Activity in 4d-Transition-Metal-Doped g-C₃N₄ Monolayers

Work Function‐Guided Electrocatalyst Design

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Theoretical inspection of TM-P4C single-atom electrocatalysts: High performance for oxygen reduction and evolution reactions

Cited by 7 publications

References 58 publications

Theoretical prediction of emerging high-performance trifunctional ORR/OER/HER single-atom catalysts: transition metals anchored into π–π conjugated graphitic carbon nitride (g-C10N3)

Theoretical prediction of emerging high-performance trifunctional ORR/OER/HER single-atom catalysts: transition metals anchored into π–π conjugated graphitic carbon nitride (g-C10N3)

Theoretical Insights on the Charge State and Bifunctional OER/ORR Electrocatalyst Activity in 4d-Transition-Metal-Doped g-C3N4 Monolayers

Work Function‐Guided Electrocatalyst Design

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Theoretical prediction of emerging high-performance trifunctional ORR/OER/HER single-atom catalysts: transition metals anchored into π–π conjugated graphitic carbon nitride (g-C₁₀N₃)

Theoretical prediction of emerging high-performance trifunctional ORR/OER/HER single-atom catalysts: transition metals anchored into π–π conjugated graphitic carbon nitride (g-C₁₀N₃)

Theoretical Insights on the Charge State and Bifunctional OER/ORR Electrocatalyst Activity in 4d-Transition-Metal-Doped g-C₃N₄ Monolayers