Synthesis and Active Site Identification of Fe−N−C Single‐Atom Catalysts for the Oxygen Reduction Reaction

Wan, Xin; Chen, Weiqi; Yang, Jiarui; Liu, Mengchan; Liu, Xiaofang; Shui, Jianglan

doi:10.1002/celc.201801302

Cited by 71 publications

(37 citation statements)

References 115 publications

(69 reference statements)

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“…In recent years, with advancements in both atomic-resolution characterization techniques and synthesis techniques, singleatom catalysts (SACs) have become one of the frontiers of PGM-free catalysts [72][73][74][75] . This class of catalysts may have relatively pure catalytic sites that are good for the fundamental research of PGM-free catalysts.…”

Section: Activity Progressed Referring To Doe Volumetric Activity Targetmentioning

confidence: 99%

Fe-N-C catalysts for PEMFC: Progress towards the commercial application under DOE reference

Wang

Wan

Liu

et al. 2019

Journal of Energy Chemistry

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Section: Activity Progressed Referring To Doe Volumetric Activity Targetmentioning

confidence: 99%

Fe-N-C catalysts for PEMFC: Progress towards the commercial application under DOE reference

Wang

Wan

Liu

et al. 2019

Journal of Energy Chemistry

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“…Although the challenge of scalability is not always taken in account, some recent approaches to limit the ion mobility show very promising results; however, since all pyrolytic approaches are based on kinetic stabilization only, the active site density is usually pretty low, with Fe contents typically not exceeding 3 wt%. [12][13][14] In more than 30 years of research, no successful preparation of ORR-active Fe-N-Cs was reported based on the coordination of iron to metal-free nitrogen-doped carbons (NDCs). Obviously, the likelihood of randomly occurring N 4 coordination sites is very low, so that Fe ions will, normally, only be loosely bound to the NDC surface (Scheme 1B).…”

Section: Introductionmentioning

confidence: 99%

Active‐Site Imprinting: Preparation of Fe–N–C Catalysts from Zinc Ion–Templated Ionothermal Nitrogen‐Doped Carbons

Menga

Ruiz‐Zepeda

Moriau

et al. 2019

Advanced Energy Materials

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sales of light electric vehicles (battery electric vehicles and plug-in hybrid electric vehicles) are politically pushed and increasing exponentially. [1] Vehicles based on proton-exchange-membrane fuel cells (PEMFCs) have the potential to surpass the limitations of battery-based ones, especially, regarding the driving range. Unfortunately, the mass commercialization of this technology is hampered by the limited availability and high cost of Pt, which is required to speed up the anodic and cathodic reactions happening in a PEMFC. [2,3] Since ≈4 times more Pt is required on the cathode than at the anode side, the development of cathode materials containing low Pt amount is a promising way to reduce costs. Unfortunately, low-Pt cathode materials suffer from other limitations, such as losses due to mass transport; [4] also, when the Pt content is reduced below 100 µg cm −2 , the cost of other components rises. [3] For these reasons, completely replacing the Pt at the cathode side is a reasonable and promising way to go.In the last 10 years, platinum-group-metal-free (PGM-free) catalysts for the oxygen reduction reaction (ORR) have drawn the attention of many research groups all over the world. Since it has been shown that bioinspired metal-nitrogen-doped-carbon (M-N-C, M = Fe, Co) catalysts could meet the requirements for Atomically dispersed Fe-N-C catalysts are considered the most promising precious-metal-free alternative to state-of-the-art Pt-based oxygen reduction electrocatalysts for proton-exchange membrane fuel cells. The exceptional progress in the field of research in the last ≈30 years is currently limited by the moderate active site density that can be obtained. Behind this stands the dilemma of metastability of the desired FeN 4 sites at the high temperatures that are believed to be a requirement for their formation. It is herein shown that Zn 2+ ions can be utilized in the novel concept of active-site imprinting based on a pyrolytic template ion reaction throughout the formation of nitrogen-doped carbons. As obtained atomically dispersed Zn-N-Cs comprising ZnN 4 sites as well as metal-free N 4 sites can be utilized for the coordination of Fe 2+ and Fe 3+ ions to form atomically dispersed Fe-N-C with Fe loadings as high as 3.12 wt%. The Fe-N-Cs are active electocatalysts for the oxygen reduction reaction in acidic media with an onset potential of E 0 = 0.85 V versus RHE in 0.1 m HClO 4 . Identical location atomic resolution transmission electron microscopy imaging, as well as in situ electrochemical flow cell coupled to inductively coupled plasma mass spectrometry measurements, is employed to directly prove the concept of the active-site imprinting approach.

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“…The development of sustainable energy technology of fuel cells and metal‐air batteries, relies on the high‐performance and cost‐effective oxygen reduction reaction (ORR) catalysts [1–3] . The platinum‐based nanomaterials possess high activity in catalyzing the ORR in acidic environment [1,4–5] . However, limited by high cost and scarce resources, large‐scale application of Pt is unrealistic.…”

Section: Introductionmentioning

confidence: 99%

“…Nitrogen‐coordinated transition metal sites (M−N x , M=Fe, Co, Ni, Mn, etc.) on carbon support have been proved to be a promising type of low‐cost ORR catalysts [1–2,8–9] . However, their intrinsic activity is still inferior to the Pt counterparts in acid electrolytes, and more types of active sites need be explored.…”

Section: Introductionmentioning

confidence: 99%

Recent Advances in Phosphorus‐Coordinated Transition Metal Single‐Atom Catalysts for Oxygen Reduction Reaction

et al. 2020

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Carbon‐supported heteroatom‐coordinated metal single‐atom catalysts (SACs) are promising electrocatalysts for oxygen reduction reaction (ORR) due to their low cost and tunable catalytic activity. Adjusting the electronic structure of the active center is an effective way to improve the activity of SACs. Compared with the intensively studied nitrogen‐coordinated transition metal atoms (e. g. Fe, Co and Mn), phosphorus‐coordinated and nitrogen‐phosphorus dual‐coordinated ones exhibit different electronic structures, which changes the reaction energy barrier and enhances the catalytic activity. This review summarizes recent advances in phosphorus coordination SACs for ORR in terms of theoretical study, site structure determination, synthesis method and catalytic activity. Further research is called for to explore the precise synthesis of phosphorus coordination SACs in a controllable manner and check the SACs under actual working conditions.

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Synthesis and Active Site Identification of Fe−N−C Single‐Atom Catalysts for the Oxygen Reduction Reaction

Cited by 71 publications

References 115 publications

Fe-N-C catalysts for PEMFC: Progress towards the commercial application under DOE reference

Fe-N-C catalysts for PEMFC: Progress towards the commercial application under DOE reference

Active‐Site Imprinting: Preparation of Fe–N–C Catalysts from Zinc Ion–Templated Ionothermal Nitrogen‐Doped Carbons

Recent Advances in Phosphorus‐Coordinated Transition Metal Single‐Atom Catalysts for Oxygen Reduction Reaction

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