N-Doped Graphene-Coated Commercial Pt/C Catalysts toward High-Stability and Antipoisoning in Oxygen Reduction Reaction

Liu, Depei; Zhang, Jie; Liu, Duanduan; Li, Taozhu; Yan, Yuandong; Wei, Xinying; Yang, Yandong; Yan, Shicheng; Zou, Zhigang

doi:10.1021/acs.jpclett.1c04005

Cited by 25 publications

(18 citation statements)

References 48 publications

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“…To alleviate catalyst deactivation, introduction of a barrier on active Pt NPs has recently been highlighted as a promising strategy. − It has been proposed that encapsulation of Pt NPs with thin layers has the potential to prevent their dissolution, detachment, and agglomeration. For instance, covering Pt NPs with a silica layer led to an enhanced durability of the Pt NPs, as supported by the insignificant changes in both the electrochemical active surface area (ECSA) and particle size after >1000 cycles of the accelerated durability test (ADT) .…”

Section: Introductionmentioning

confidence: 99%

“…This is because of the unavoidable blockage of the active Pt surface and the reduction in the fraction of exposed Pt sites. However, such prospects have often been disproved based on the almost comparable or even better ORR activity of fresh C@Pt/C catalysts than that of carbon-free Pt/C. − ,− ,, …”

Section: Introductionmentioning

confidence: 99%

“…Several hypotheses have been proposed to rationalize the above-mentioned counterintuitive phenomena. − ,− ,, As the main catalytic sites, the Pt sites in C@Pt/C are considered responsible for ORR activity, − ,− and possible modification of the intrinsic catalytic activity (i.e., turnover) of the Pt NPs has been suggested to be induced by their interaction with the carbon layers. ,− Moreover, the formation of the carbon layer at the Pt surface can prevent the undesirable poisoning of sulfonate from the ionomer, resulting in enhanced activity and durability in the fuel cell device . In contrast, it has been proposed that the Pt NPs buried under the carbon layers are assumed as spectators (or promotors) and their carbon shell functions as the main catalytic site for the ORR. ,, The latter suggestion is typically for C@Pt/C catalysts with heteroatom moieties (e.g., N, S, etc.) owing to the considerable ORR activity of metal-free heteroatom-doped carbons. ,,, However, identical conclusion was also derived for heteroatom-free C@Pt/C catalysts .…”

Section: Introductionmentioning

confidence: 99%

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Does the Encapsulation Strategy of Pt Nanoparticles with Carbon Layers Really Ensure Both Highly Active and Durable Electrocatalysis in Fuel Cells?

Kwon²,

Kim

et al. 2022

ACS Catal.

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Platinum is a key component of commercialized proton exchange membrane fuel cells (PEMFCs) to lower the energy cost of the sluggish oxygen reduction reaction (ORR) at the cathode. Beyond the significant advances in improving its initial activity, securing catalytic durability is the next challenge for the successful implementation of PEMFCs. Encapsulation of Pt nanoparticles (NPs) with thin carbon or silica layers has recently been highlighted as a promising strategy for alleviating Pt degradation. However, unexpectedly similar or occasionally even better catalytic activity on site-blocked Pt NPs has raised fundamental interest about the nature of their catalytic sites and the origin of the prolonged durability. Herein, to answer these questions, we investigate the ORR and methanol oxidation reaction activities of carbon-encapsulated Pt NP (C@Pt/C) catalysts. By controlling the robustness of the carbon shells synthetically and electrochemically, directly exposed Pt sites, at which facile transport of reactant/ product molecules occurs via the loosely packed or highly defective carbon layers, are identified as the main catalytic sites. Interestingly, online differential electrochemical mass spectroscopy and inductively coupled plasma-mass spectrometry coupled to electrochemical flow cells verify a trade-off relationship between the activity and stability of the catalysts. In addition to their role as a physical barrier for prohibiting the dissolution and agglomeration of the Pt NPs, the carbon shell acts as a sacrificial agent, questioning the practical legitimacy of the strategy for achieving both high activity and durability.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Does the Encapsulation Strategy of Pt Nanoparticles with Carbon Layers Really Ensure Both Highly Active and Durable Electrocatalysis in Fuel Cells?

Kwon²,

Kim

et al. 2022

ACS Catal.

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“…Therefore, efficient catalysts must be developed to increase the reaction rate [ 18 , 19 , 20 ]. At present, commercial precious metal Pt-based materials are considered to effectively catalyze the ORR; however, they are limited by high cost and poor stability [ 21 , 22 , 23 ]. Therefore, we consider enhancing the applicability of the catalysts in terms of reducing the cost and improving catalyst stability to increase their efficiency in the ORR.…”

Section: Introductionmentioning

confidence: 99%

Evaluating the Growth of Ceria-Modified N-Doped Carbon-Based Materials and Their Performance in the Oxygen Reduction Reaction

Chang

Jia

2022

Nanomaterials

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Owning to their distinctive electronic structure, rare-earth-based catalysts exhibit good performance in the oxygen reduction reaction (ORR) and can replace commercial Pt/C. In this study, CeO2-modified N-doped C-based materials were synthesized using salt template and high-temperature calcination methods, and the synthesis conditions were optimized. The successful synthesis of CeO2–CN–800 was confirmed through a series of characterization methods and electrochemical tests. The test results show that the material has the peak onset potential of 0.90 V and the half-wave potential of 0.84 V, and has good durability and methanol resistance. The material demonstrates good ORR catalytic performance and can be used in Zn–air batteries. Moreover, it is an excellent catalyst for new energy equipment.

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“…With an increasing demand for the green and renewable energy technologies, the hydrogen evolution reaction (HER) and the oxygen reduction reaction (ORR) have drawn intensive attention as they are crucial for numerous energy conversion and storage devices, such as electrolyzers, fuel cells, and rechargeable batteries. − However, general high overpotentials and sluggish kinetics of HER and ORR processes have hampered large-scale practical implementations of these sustainable energy technologies. − Therefore, it is imperative to search for effective catalysts to reduce the energy barriers and enhance the catalytic efficiency of these fundamental reactions …”

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 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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N-Doped Graphene-Coated Commercial Pt/C Catalysts toward High-Stability and Antipoisoning in Oxygen Reduction Reaction

Cited by 25 publications

References 48 publications

Does the Encapsulation Strategy of Pt Nanoparticles with Carbon Layers Really Ensure Both Highly Active and Durable Electrocatalysis in Fuel Cells?

Does the Encapsulation Strategy of Pt Nanoparticles with Carbon Layers Really Ensure Both Highly Active and Durable Electrocatalysis in Fuel Cells?

Evaluating the Growth of Ceria-Modified N-Doped Carbon-Based Materials and Their Performance in the Oxygen Reduction Reaction

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

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