Room-Temperature Methane Conversion by Graphene-Confined Single Iron Atoms

Cui, Xiaoju; Li, Haobo; Wang, Yan; Hu, Yuanli; Lee, Hua; Li, Haiyang; Han, Xiuwen; Liu, Qingfei; Yang, Fan; He, Limin; Chen, Xiaoqi; Li, Qingyun; Xiao, Jianping; Deng, Dehui; Bao, Xinhe

doi:10.1016/j.chempr.2018.05.006

Cited by 402 publications

(361 citation statements)

References 37 publications

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“…In addition to the electrocatalytic reactions mentioned above, SACs have also been reported to be used in other catalytic reactions, including NRR, WGSR, methane reforming, methanol steam reforming, CO oxidation, benzene oxidation, acetylene hydrogenation, and so on. Shan et al reported an atomically dispersed Rh on the zeolite (Rh/ZSM‐5) catalyst, which can convert methane into methanol or acetic acid in liquid phase mild oxidation at 150 °C.…”

Section: Recent Advances Of Densely Populated Sacs In Catalytic Applimentioning

confidence: 99%

Densely Populated Single Atom Catalysts

et al. 2019

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Developing highly efficient electrocatalysts with low cost is critical for the wide‐spread application of sustainable and renewable energy conversion technologies. Single‐atom catalysts (SACs) have attracted considerable attention owing to their high catalytic activity, selectivity, and stability. However, the high surface energy of the single atoms often results in an extremely low loading of metal atom catalysts with limited mass activity. In this context, densely populated SACs are more promising for practical applications due to their high active surface area and mass activity. Herein, the recent research progress of high loading (≥5 wt%) SACs for different electrocatalytic applications is summarized. An overview of various synthesis and characterization strategies of SACs is presented in this review. The influence of appropriate substrates on the preparation of high metal loading SACs is also discussed. In addition, this review provides valuable insights into the current challenges and future opportunities in the field of single‐atom catalysts.

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Section: Recent Advances Of Densely Populated Sacs In Catalytic Applimentioning

confidence: 99%

Densely Populated Single Atom Catalysts

et al. 2019

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“…The adjacent carbon atoms of FeN 4 center were also reconstructed with the high energy, leading to the dispersed single Fe atoms embedded into the defects of graphene (FeN 4 /GN) (Figure e,f). The unsaturated Fe sites of FeN 4 /GN possess the unsaturated FeN bonds, which exhibit high activity in catalyzing the oxidation reaction such as the oxidation of benzene to phenol and methane to C1 oxygenated products at room temperature . Therefore, high energy ball milling synthesis is a promising strategy to fabricate a variety of atomic metal catalysts on graphene without any extra external energy supply.…”

Section: Fabrication Strategies and Characteristic Methods Of Sagmentioning

confidence: 99%

“…Moreover, the formation of the extraordinary OFeN 4 O structure improves the electrocatalytic activity of the CH bond for forming the methyl radical at a low reaction energy barrier of 0.79 eV. In addition, the OFeN 4 O active sites could break the CH bonds of methane and directly convert it into C1 oxygenated products at 25 °C in methane oxidation process . Therefore, with the increasing of time, the products are almost CH 3 OH and CH 3 OOH in the first 100 min and then HOCH 2 OOH and HCOOH (Figure e).…”

Section: Electrochemical Applications Of Sagmentioning

confidence: 98%

“…Because of the high reserves and low cost, methane is one of the most chemical feed stocks for producing methanol, olefins, and dimethyl ether and so on. However, the activation of methane is limited by the stable and inert hydrocarbon with ∆ H C  H = 104 kcal mol −1 , which greatly suppresses its practical application in many fields . To improve the sluggish activity, the key is to activate the inert CH bond in methane.…”

Section: Electrochemical Applications Of Sagmentioning

confidence: 99%

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Single Atoms on Graphene for Energy Storage and Conversion

et al. 2019

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Single atoms are attracting much attention in the field of energy conversion and storage due to their maximal atomic utilization, high efficiency, and good selectivity. Moreover, their unique electronic structure could improve the intrinsic activity of the active sites. However, the high surface free energy of single atoms inevitably results in their serious aggregation, leading to degraded catalytic activity and poor cycling life. To solve these issues, supports with high surface areas have to be developed to reduce loading density of single atoms and further decrease the surface free energy. Furthermore, engineering the active sites of these substrates can also regulate chemical coordination of single atoms, enhancing their catalytic performance. Owing to high surface area, excellent conductivity and adjustable surface properties, graphene is widely utilized to load atomic metal catalysts. In this review, the fabrication strategies and characterization methods of single atoms on graphene (SAG) are summarized first. Subsequently, the electrochemical applications of SAG on the oxygen reduction reaction, oxygen evolution reaction, hydrogen evolution reaction, carbon dioxide reduction, and methane oxidation are discussed in detail. Finally, the future developments and prospects in fabrication and application of SAG are also discussed.

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“…[66][67][68] Auch Heterogenkatalysatoren kçnnen Methan zu Methanol umwandeln, z. Erst kürzlich wurden ein kolloidaler PdAu-Katalysator, [74] trägerfixierte Rh-Katalysatoren [76] und ein Graphen-eingeschränkter Einzelatom-Fe-Katalysator [75] entwickelt, die CH 4 auch bei tiefen Te mperaturen wirkungsvoll zu Methanol umwandeln konnten. [72,73] Bei diesem Verfahren sind hohe Reaktionstemperaturen (400-800 K) und -drücke (20-70 bar) erforderlich, um vernünftige Methan-Umwandlungsgeschwindigkeiten zu erzielen.…”

Section: Aufsätzeunclassified

Von Sonnenlicht zu Brennstoffen: aktuelle Fortschritte der C₁‐Solarchemie

et al. 2019

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Die katalytische C1‐Chemie auf der Grundlage der Aktivierung/Umwandlung von Synthesegas (CO+H2), Methan, Kohlendioxid und Methanol verfügt über enormes Potential für die Entwicklung nachhaltiger Kohlenwasserstoffbrennstoffe als Ersatz für Öl, Kohle und Erdgas. Herkömmliche thermisch‐katalytische Verfahren zur C1‐Umsetzung benötigen hohe Temperaturen und Drücke und sind daher mit einem großen CO2‐Fußabdruck verbunden. Dagegen bietet die solargetriebene C1‐Katalyse einen umweltfreundlichen und nachhaltigen Weg für die Herstellung von Brennstoffen und anderen chemischen Grundstoffen, wenn auch die Umwandlungseffizienzen noch zu niedrig für industrielle Wirtschaftlichkeit sind. In unserem Aufsatz beleuchten wir aktuelle Fortschritte und Meilensteine der C1‐Solarchemie, einschließlich der solaren Fischer‐Tropsch‐Synthese, Wassergas‐Shift‐Reaktion, CO2‐Hydrierung, Methan‐ und Methanolumwandlung. Ein besonderer Schwerpunkt liegt auf der rationalen Entwicklung von Katalysatoren, Struktur‐Reaktivitäts‐Beziehungen und Reaktionsmechanismen. Strategien für die Hochskalierung solargetriebener C1‐Verfahren werden ebenfalls diskutiert.

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Room-Temperature Methane Conversion by Graphene-Confined Single Iron Atoms

Cited by 402 publications

References 37 publications

Densely Populated Single Atom Catalysts

Densely Populated Single Atom Catalysts

Single Atoms on Graphene for Energy Storage and Conversion

Von Sonnenlicht zu Brennstoffen: aktuelle Fortschritte der C₁‐Solarchemie

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Room-Temperature Methane Conversion by Graphene-Confined Single Iron Atoms

Cited by 402 publications

References 37 publications

Densely Populated Single Atom Catalysts

Densely Populated Single Atom Catalysts

Single Atoms on Graphene for Energy Storage and Conversion

Von Sonnenlicht zu Brennstoffen: aktuelle Fortschritte der C1‐Solarchemie

Contact Info

Product

Resources

About

Von Sonnenlicht zu Brennstoffen: aktuelle Fortschritte der C₁‐Solarchemie