Hierarchical porous single-wall carbon nanohorns with atomic-level designed single-atom Co sites toward oxygen reduction reaction

Jung, Jae Young; Kim, Sungjun; Kim, Jeong-Gil; Kim, Min Ji; Lee, Kug‐Seung; Sung, Yung‐Eun; Kim, Pil; Yoo, Sung Jong; Lim, Hyung‐Kyu; Kim, Nam Dong

doi:10.1016/j.nanoen.2022.107206

Cited by 24 publications

(21 citation statements)

References 46 publications

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“…37 Very recently, with the combination of DC arc discharge and thermal annealing, a hierarchical carbon nanohorns with Co−N x sites has been developed. 38 These all demonstrate the fabrication feasibility of our designed catalysts.…”

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confidence: 54%

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Utilizing High Coordination Diversity in Carbon Nanocone Supported Catalytic Single-Atom Sites for Screening of Optimal Activity

Deng

Zhang

et al. 2022

J. Phys. Chem. Lett.

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The hydrogen evolution reaction (HER) and the oxygen reduction reaction (ORR) are crucial in various energy conversion and storage technologies. Performances of catalysts are appreciably affected by the adsorption energies of key reaction intermediates, whereas the active site engineering to achieve optimal adsorption energy remains challenging. Herein, using density functional theory calculations, we proposed a novel design of transition metal single-atom active sites supported by carbon nanocone (CNC) with high coordination diversity. The particularly diversified electronic states of CNC carbon atoms endow varying coordination to the metal active sites, which then results in a near-continuum distribution of adsorption energies for key intermediates. With this mode, 33 CNC-based active sites exhibit outstanding catalytic potential for the HER with near-zero free energy barriers. Meanwhile, five distinct Cu−N 3 active sites can serve as promising candidates for the ORR with low overpotentials. Our work suggests a new strategy of making nanocone-based single-atom catalysts with promising catalytic performance.

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confidence: 54%

“…The nickel loading could be further improved with an additional chemical etching of nitrogen doped graphene materials . Very recently, with the combination of DC arc discharge and thermal annealing, a hierarchical carbon nanohorns with Co–N x sites has been developed . These all demonstrate the fabrication feasibility of our designed catalysts.…”

mentioning

confidence: 99%

Utilizing High Coordination Diversity in Carbon Nanocone Supported Catalytic Single-Atom Sites for Screening of Optimal Activity

Deng

Zhang

et al. 2022

J. Phys. Chem. Lett.

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“…The authors also demonstrated the considerable electrocatalytic ORR performance of Co@MCM under acidic conditions. Besides, Jung et al recently synthesized a Co-N 4 sites decorated single-wall carbon nanohorns catalyst via an ammonia annealing process for efficient electrocatalytic ORR [ 91 ]. By employing DFT calculations, they attributed the high intrinsic electrocatalytic ORR activity of the Co-N 4 catalyst to a ligand-push effect of water molecules to the Co-N 4 sites in the axial direction.…”

Section: Regulation Of the First Coordination Shellmentioning

confidence: 99%

Rational coordination regulation in carbon-based single-metal-atom catalysts for electrocatalytic oxygen reduction reaction

Cui

Gao

et al. 2022

Nano Convergence

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Single-metal-atom catalysts (SMACs) have garnered extensive attention for various electrocatalytic applications, owing to their maximum atom-utilization efficiency, tunable electronic structure, and remarkable catalytic performance. In particular, carbon-based SMACs exhibit optimal electrocatalytic activity for the oxygen reduction reaction (ORR) which is of paramount importance for several sustainable energy conversion and generation technologies, such as fuel cells and metal-air batteries. Despite continuous endeavors in developing various advanced carbon-based SMACs for electrocatalytic ORR, the rational regulation of coordination structure and thus the electronic structure of carbon-based SMACs remains challenging. In this review, we critically examine the role of coordination structure, including local coordination structure (i.e., metal atomic centers and the first coordination shell) and extended local coordination structure (i.e., the second and higher coordination shells), on the rational design of carbon-based SMACs for high-efficiency electrocatalytic ORR. Insights into the relevance between coordination structures and their intrinsic ORR activities are emphatically exemplified and discussed. Finally, we also propose the major challenges and future perspectives in the rational design of advanced carbon-based SMACs for electrocatalytic ORR. This review aims to emphasize the significance of coordination structure and deepen the insightful understanding of structure-performance relationships.

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“…On the other hand, to the best of our knowledge, the surface curvature effect that enhances dual-atom site catalysis and goes beyond the scaling relations remains unknown. Porous carbon materials, such as M–N–Cs, are ideal candidates to investigate this effect because they are inherently curved. − A significant fraction of double-atom sites among randomly distributed single-atom sites is visible in many M–N–C materials, for example, in microscopic images. − Hypothetically, optimizing the surface curvature and intersite distance of M–N–Cs can change the reaction mechanism and increase the OER/ORR activity.…”

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confidence: 99%

Surface Curvature Effect on Dual-Atom Site Oxygen Electrocatalysis

2023

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Improved oxygen electrocatalysis is crucial for the ever-growing energy demand. Metal–nitrogen-carbon (M–N–C) materials are promising candidates for catalysts. Their activity is tunable via varying electronic and geometric properties, such as porosity. Because of the difficulty in modeling porosity, M–N–Cs with variable surface curvature remained largely unexplored. In this work, we developed a realistic in-pore dual-atom site M–N–C model and applied density functional theory to investigate the surface curvature effect on oxygen reduction and evolution reactions. We show that surface curving tailors both scaling relations and energy barriers. Thus, we predict that adjusting the surface curvature can improve the catalytic activity toward mono- and bifunctional oxygen electrocatalysis.

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Hierarchical porous single-wall carbon nanohorns with atomic-level designed single-atom Co sites toward oxygen reduction reaction

Cited by 24 publications

References 46 publications

Utilizing High Coordination Diversity in Carbon Nanocone Supported Catalytic Single-Atom Sites for Screening of Optimal Activity

Utilizing High Coordination Diversity in Carbon Nanocone Supported Catalytic Single-Atom Sites for Screening of Optimal Activity

Rational coordination regulation in carbon-based single-metal-atom catalysts for electrocatalytic oxygen reduction reaction

Surface Curvature Effect on Dual-Atom Site Oxygen Electrocatalysis

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