Atomically dispersed Fe-Cu dual-site catalysts synergistically boosting oxygen reduction for hydrogen fuel cells

Xiao, Zeyu; Sun, Panpan; Qiao, Zelong; Qiao, Kangwei; Xu, Haoxiang; Wang, Shitao; Cao, Dapeng

doi:10.1016/j.cej.2022.137112

Cited by 74 publications

(42 citation statements)

References 65 publications

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“…Computational framework used to systematically study DMSCs for their catalytic activity toward ORR. On the right top, SEM image of experimentally synthesized DMSCs; middle right, HAADF-STEM to identify dual-atom clusters (red) and single atoms (yellow); bottom right, rotating disk electrode to show the ORR performances of as-synthesized DMSCs . Reprinted from Chemical Engineering Journal, 446, 137112, 2022, with permission from Elsevier.…”

Section: Resultsmentioning

confidence: 99%

Mechanistic Insight into Dual-Metal-Site Catalysts for the Oxygen Reduction Reaction

Brea

2023

ACS Catal.

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Incorporating a second transition metal to iron− nitrogen−carbon single-atom catalysts (Fe−N−C SACs) to design dual-metal-site catalysts (DMSCs) was demonstrated to offer a promising opportunity to enhance the oxygen reduction reaction (ORR). However, due to the many possible structural configurations and the dynamic structure evolution of metal centers under reaction conditions, it is challenging to clearly elucidate the structure−property relationship at the atomic level. Here, we develop a computational workflow integrating configuration generations, phase diagram constructions, and reaction free energy calculations to provide an insightful understanding of the active site structures and catalytic mechanisms of ORR on DMSCs. Using Fe−Cu as an example, we generate 31 configurations by tiling the hexagonal lattice of graphene and investigate their atomic structures under reaction conditions. We find that for a wide range of electrode potentials, the Fe site is covered by an *OH intermediate, while the Cu site is not covered by any intermediate. With the OH-ligated structures, we identify the configurations which possess higher catalytic activity than Fe−N−C and Pt(111). We demonstrate that ORR on Fe−Cu DMSCs proceeds via the associative pathway, and the desorption of *OH is the rate-determining step. Further analysis reveals a linear correlation between the limiting potential and the magnetic moment on Fe and suggests a closer distance between the two metal sites benefits the catalytic activity. These mechanistic insights pave the way for the rational design of efficient platinum group metal-free DMSCs for ORR.

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Section: Resultsmentioning

confidence: 99%

Mechanistic Insight into Dual-Metal-Site Catalysts for the Oxygen Reduction Reaction

Brea

2023

ACS Catal.

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“…It can be easily found that Fe is coordinated with O due to the clear COHP line, and coincides with some of the PDOS peak. [ 48 ] All the bonding orbitals are below the Fermi level, indicating their strong and stable coordination bonds between Fe ions and HATNTA. [ 49 , 50 ]…”

Section: Resultsmentioning

confidence: 99%

High‐Rate Organic Cathode Constructed by Iron‐Hexaazatrinaphthalene Tricarboxylic Acid Coordination Polymer for Li‐Ion Batteries

et al. 2022

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The sluggish ion-transport in electrodes and low utilization of active materials are critical limitations of organic cathodes, which lead to the slow reaction dynamics and low specific capacity. In this study, the hierarchical tube is constructed by iron-hexaazatrinaphthalene tricarboxylic acid coordination polymer (Fe-HATNTA), using HATNTA as the self-engaged template to coordinate with Fe 2+ ions. This Fe-HATNTA tube with hierarchical porous structure ensures the sufficient contact between electrolyte and active materials, shortens the diffusion distance, and provides more favorable transport pathways for ions. When employed as the cathode for rechargeable Li-ion batteries, Fe-HATNTA delivers a high specific capacity (244 mAh g −1 at 50 mA g −1 , 91% of theoretical capacity), excellent rate capability (128 mAh g −1 at 9 A g −1 ), and a long-term cycle life (73.9% retention over 3000 cycles at 5 A g −1 ). Moreover, the Li + ions storage and conduction mechanisms are further disclosed by the ex situ and in situ characterizations, kinetic analyses, and theoretical calculations. This work is expected to boost further enthusiasm for developing the hierarchical structured metal-organic coordination polymers with superb ionic storage and transport as high-performance organic cathodes.

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“…6b). The free energy diagram 56,57 for the oxygen intermediates based on the 4e À path (Fig. 6d, S23 and Table S5 †) clearly shows that the Co(111) (0.275 V) and Fe 2 P(111) (À0.196 V) crystals surfaces have relatively poor ORR activity, due to the excessively strong adsorption.…”

Section: Resultsmentioning

confidence: 99%

Facile synthesis of Fe₂P/Co embedded trifunctional electrocatalyst for high-performance anion exchange membrane fuel cells, rechargeable Zn–air batteries, and overall water splitting

et al. 2022

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Atomically dispersed Fe-Cu dual-site catalysts synergistically boosting oxygen reduction for hydrogen fuel cells

Cited by 74 publications

References 65 publications

Mechanistic Insight into Dual-Metal-Site Catalysts for the Oxygen Reduction Reaction

Mechanistic Insight into Dual-Metal-Site Catalysts for the Oxygen Reduction Reaction

High‐Rate Organic Cathode Constructed by Iron‐Hexaazatrinaphthalene Tricarboxylic Acid Coordination Polymer for Li‐Ion Batteries

Facile synthesis of Fe₂P/Co embedded trifunctional electrocatalyst for high-performance anion exchange membrane fuel cells, rechargeable Zn–air batteries, and overall water splitting

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Atomically dispersed Fe-Cu dual-site catalysts synergistically boosting oxygen reduction for hydrogen fuel cells

Cited by 74 publications

References 65 publications

Mechanistic Insight into Dual-Metal-Site Catalysts for the Oxygen Reduction Reaction

Mechanistic Insight into Dual-Metal-Site Catalysts for the Oxygen Reduction Reaction

High‐Rate Organic Cathode Constructed by Iron‐Hexaazatrinaphthalene Tricarboxylic Acid Coordination Polymer for Li‐Ion Batteries

Facile synthesis of Fe2P/Co embedded trifunctional electrocatalyst for high-performance anion exchange membrane fuel cells, rechargeable Zn–air batteries, and overall water splitting

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Facile synthesis of Fe₂P/Co embedded trifunctional electrocatalyst for high-performance anion exchange membrane fuel cells, rechargeable Zn–air batteries, and overall water splitting