Tailoring the electrocatalytic oxygen reduction reaction pathway by tuning the electronic states of single-walled carbon nanotubes

Hu, Ronggui; Wu, Chuxin; Hou, Kun; Xia, Chenmaya; Yang, Juan; Guan, Lunhui; Li, Yan

doi:10.1016/j.carbon.2019.02.067

Cited by 18 publications

(10 citation statements)

References 36 publications

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“…Accordingly, this calls for further regulation of the active configuration toward optimal absorption−desorption behavior of oxygen species. 13 The critical challenge of directly measuring the intermediate adsorption properties makes the tailoring of adsorption energy at the catalytic center experimentally difficult. Fortunately, this dilemma was greatly alleviated by the finding that the Fe(III)/ Fe(II) redox potential (E redox ) is an effective M−O binding energy indicator, where higher E redox suggests weaker Fe−O binding strength.…”

Section: ■ Introductionmentioning

confidence: 99%

Climbing the Apex of the ORR Volcano Plot via Binuclear Site Construction: Electronic and Geometric Engineering

et al. 2019

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Great enthusiasm in single-atom catalysts (SACs) for the oxygen reduction reaction (ORR) has been aroused by the discovery of M−N X as a promising ORR catalysis center. However, the performance of SACs lags far behind that of stateof-the-art Pt due to the unsatisfactory adsorption−desorption behaviors of the reported catalytic centers. To address this issue, rational manipulation of the active site configuration toward a well-managed energy level and geometric structure is urgently desired, yet still remains a challenge. Herein, we report a novel strategy to accomplish this task through the construction of an Fe−Co dual-atom centered site. A spontaneously absorbed electron-withdrawing OH ligand was proposed to act proactively as an energy level modifier to empower easy intermediate desorption, while the triangular Fe−Co−OH coordination facilitates O−O bond scission. Benefiting from these attributes, the as-constructed FeCoN 5 −OH site enables an ORR onset potential and half-wave potential of up to 1.02 and 0.86 V (vs RHE), respectively, with an intrinsic activity over 20 times higher than the single-atom FeN 4 site. Our finding not only opens up a novel strategy to tailor the electronic structure of an atomic site toward boosted activity but also provides new insights into the fundamental understanding of diatomic sites for ORR electrocatalysis.

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Section: ■ Introductionmentioning

confidence: 99%

Climbing the Apex of the ORR Volcano Plot via Binuclear Site Construction: Electronic and Geometric Engineering

et al. 2019

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“…Distinct from other carbon nanomaterials, CNTs show a high degree crystallinity, geometric curvature, hollow configurations, and different chirality. These features and properties can be used to effectively tailor their catalytic performance. − Moreover, many techniques, such as the furnace-moving method and water-assisted synthesis, have been developed and maybe available for large-scale production of CNT-based catalysts. , …”

Section: Introductionmentioning

confidence: 99%

Identification of Efficient Active Sites in Nitrogen-Doped Carbon Nanotubes for Oxygen Reduction Reaction

Zhou

et al. 2020

J. Phys. Chem. C

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Nitrogen-doped carbon nanotubes (NCNTs) have demonstrated great promise as an electrocatalyst alternative to platinum for oxygen reduction reaction (ORR). However, there is much disagreement regarding which N doping sites are most desirable for the reaction. Here, we report an experimental and computational study to identify the efficient active sites in NCNTs for ORR in alkaline media. In our experiments, we synthesized NCNTs of similar overall N content (∼4.1%) and carbon matrix but varying percentages of different types of N doping species. Our results reveal a positive correlation between ORR activity and the content of graphitic N doping. Furthermore, we performed density functional theory calculations to predict the free energy evolution of ORR on various N doping sites in NCNTs. Our computational results also indicate that graphitic N doping sites exhibit higher thermodynamic limiting potential for ORR than pyridinic N doping sites. Our combined experimental and theoretical study concludes that graphitic N doping sites are more efficient for ORR than pyridinic N doping in NCNTs.

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“…Moreover, SWCNTs were able to store hydrogen within their pores, which was confirmed through the galvanostatic charge-discharge method. Hu's group [110] found that enclosing catalytically active potassium and iron metal nanoparticles in SWCNT catalysts improves ORR electrocatalytic activity. Further, Wu and Xu [111] showed that in comparison with the assembly using Pt supported on both MWCNT and SWCNT electrodes, during the electrochemical oxidation of methanol, Pt-SWCNT/NAF catalyst displayed significantly enhanced power density, lower onset potential, and lower R CT values using CV and EIS analysis, whereas Pt-MWCNT/NAF catalysts displayed higher tolerance to CO poisoning and richness in oxygen-containing functional groups.…”

Section: Single-walled Carbon Nanotube-based Materialsmentioning

confidence: 99%

Recent Developments in Carbon-Based Nanocomposites for Fuel Cell Applications: A Review

et al. 2022

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Carbon-based nanocomposites have developed as the most promising and emerging materials in nanoscience and technology during the last several years. They are microscopic materials that range in size from 1 to 100 nanometers. They may be distinguished from bulk materials by their size, shape, increased surface-to-volume ratio, and unique physical and chemical characteristics. Carbon nanocomposite matrixes are often created by combining more than two distinct solid phase types. The nanocomposites that were constructed exhibit unique properties, such as significantly enhanced toughness, mechanical strength, and thermal/electrochemical conductivity. As a result of these advantages, nanocomposites have been used in a variety of applications, including catalysts, electrochemical sensors, biosensors, and energy storage devices, among others. This study focuses on the usage of several forms of carbon nanomaterials, such as carbon aerogels, carbon nanofibers, graphene, carbon nanotubes, and fullerenes, in the development of hydrogen fuel cells. These fuel cells have been successfully employed in numerous commercial sectors in recent years, notably in the car industry, due to their cost-effectiveness, eco-friendliness, and long-cyclic durability. Further; we discuss the principles, reaction mechanisms, and cyclic stability of the fuel cells and also new strategies and future challenges related to the development of viable fuel cells.

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Tailoring the electrocatalytic oxygen reduction reaction pathway by tuning the electronic states of single-walled carbon nanotubes

Cited by 18 publications

References 36 publications

Climbing the Apex of the ORR Volcano Plot via Binuclear Site Construction: Electronic and Geometric Engineering

Climbing the Apex of the ORR Volcano Plot via Binuclear Site Construction: Electronic and Geometric Engineering

Identification of Efficient Active Sites in Nitrogen-Doped Carbon Nanotubes for Oxygen Reduction Reaction

Recent Developments in Carbon-Based Nanocomposites for Fuel Cell Applications: A Review

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