P-doped nanomesh graphene with high-surface-area as an efficient metal-free catalyst for aerobic oxidative coupling of amines

Yang, Fan; Fan, Xiaoxu; Wang, Chunxia; Yang, Wang; Hou, Liqiang; Xu, Xiuwen; Feng, Andong; Dong, Shaojun; Chen, Kai; Wang, Ying; Li, Yongfeng

doi:10.1016/j.carbon.2017.05.101

Cited by 76 publications

(32 citation statements)

References 46 publications

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“…Monatomic layer two-dimensional (2D) materials, such as graphene, [37][38][39][40][41] g-C 3 N 4 , [42][43][44] BN, [27,[45][46][47][48] have novel properties and been already applied in wide-ranging fields. Recently, the simple 2D structure as the substrate has been doped by single TM atom, which is known as the single-atom catalysts.…”

Section: Introductionmentioning

confidence: 99%

Transition Metal‐dinitrogen Complex Embedded Graphene for Nitrogen Reduction Reaction

et al. 2019

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Conversion of nitrogen to ammonia (NH3) is one of the most important issue in the modern chemical industry. Transition metals (TM) have the special unoccupied and occupied d orbitals to accept the electrons from and backdonate to N2, which is crucial in effective nitrogen reduction reaction (NRR). Herein, we propose TMN4 (TM=Fe, Co, Mo, W, Ru, Rh) embedded graphene as the catalysts for NRR by using the density functional theory calculations. Our results revealed that MoN4 embedded graphene exhibited outstanding catalytic activity for ammonia synthesis at ambient conditions along with small reaction energy barrier of 0.67 eV, as well as against hydrogen evolution reaction. These findings provide a potential paradigm for NRR.

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Section: Introductionmentioning

confidence: 99%

Transition Metal‐dinitrogen Complex Embedded Graphene for Nitrogen Reduction Reaction

et al. 2019

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“…P‐doped carbon nanomaterials, the P is considered to be the catalytic site due to the low electronegativity value (2.19) of P compare with C (2.55) . Moreover, the carbon framework can be introduced more distortion by the P‐doping due to its larger diameter than C, which the reactivity of P‐doped carbon for catalysis of various organic reactions is enhanced ,. Recently, N and P co‐doped carbon materials have been illustrated to significantly improve their electrochemical catalysis performance owing to the increased number of dopant heteroatoms and the synergistic effects of the N and P heteroatoms ,,.…”

Section: Introductionmentioning

confidence: 99%

Nitrogen and Phosphorus Co‐Doped Graphene‐Like Carbon Catalyzed Selective Oxidation of Alcohols

Yang

Cao²,

et al. 2019

Asian J Org Chem

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The nitrogen and phosphorus co-doped graphenelike carbon (NPG) is cost-effective fabricated by simple ballmilling and thermal treatment. The as-prepared NPG can be used as a metal-free catalyst for selective catalytic oxidation of aromatic alcohols to their corresponding acids by using TBHP and O 2 as the oxidant in water. It is observed that various aromatic alcohols bearing electron-donating/withdrawing groups can be oxidized to the corresponding acids in excellent yields. No dehalogenation and steric-hindrance effects are detected in this oxidation process. In addition, the NPG catalyst can be easily separated and efficiently reused seven times, showing good recyclability.[a] Prof.for 48 h. At the end of ball milling, oxygen and nitrogen functional groups are introduced by ball milling. The final material is further Soxhlet extracted using 1 M HCl solution to eliminate metallic impurities followed by using deionized water and ethanol washing four times and drying at 80°C in the oven in 8 h.

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“…The use of N‐doped graphene for catalytic application is in the early stage, and there are some emerging exciting directions. The doping concentration, configurations strongly determine their activity, selectivity, and long‐term stability, in addition to intrinsic functional groups, defect, edges, and surface charges . But the nonstoichiometric and inhomogeneous nature of doped graphene presents daunting challenges for understanding the mechanism of intrinsic catalysis, and thus their active sites are not well understood .…”

Section: Introductionmentioning

confidence: 99%

“…This doping concentration may limit the conventional tuning of dopant types and populations at atomic levels, rendering the probing of the function of each configurations and their synergistic effects toward carbocatalysis. Furthermore, the thermal annealing process includes metal oxide, such as MgO, etc., as a template, bringing the metal impurity in resultant doped graphene . It has been frequently observed that impurities of highly active metals elements, even at the ppm level can contribute to a significant extent to the observed catalytic activity.…”

Section: Introductionmentioning

confidence: 99%

Selective Etching of N‐Doped Graphene Meshes as Metal‐Free Catalyst with Tunable Kinetics, High Activity and the Origin of New Catalytic Behaviors

Dai

Zhou

Huang

et al. 2018

Part & Part Syst Charact

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New N‐doped reduced graphene oxide (N‐RGO) meshes are facile fabricated by selective etching of 3–5 nm nanopores, with controllable doping of N dopants at an ultrahigh N/C ratio up to 15.6 at%, from pristine graphene oxide sheets in one‐pot hydrothermal reaction. The N‐RGO meshes are illustrated to be an efficient metal‐free catalyst toward hydrogenation of 4‐nitrophenol, with new catalytic behaviors emerging in following three aspects: (i) tunable kinetics following pseudofirst order from commonly observed pseudozero order; (ii) strikingly improved activity with 26‐fold increased rate constant (1.0 s−1 g−1 L); (iii) no induction time required prior to reaction due to depressed back conversion, and dramatically decreased apparent activation energy (Ea) (17 kJ mol−1). The origin of these new catalytic properties can be assigned to the synergetic effects between graphitic N doping and structural defects arising from nanopores. Deeper understanding unveils that the concentration of graphitic N is inverse proportion to Ea, while the pyrrolic N has no impact on this reaction, and oxygenate groups hampers it. The porous nature allows the N‐RGO meshes to conduct catalyze reactions in continuous flow fashion.

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P-doped nanomesh graphene with high-surface-area as an efficient metal-free catalyst for aerobic oxidative coupling of amines

Cited by 76 publications

References 46 publications

Transition Metal‐dinitrogen Complex Embedded Graphene for Nitrogen Reduction Reaction

Transition Metal‐dinitrogen Complex Embedded Graphene for Nitrogen Reduction Reaction

Nitrogen and Phosphorus Co‐Doped Graphene‐Like Carbon Catalyzed Selective Oxidation of Alcohols

Selective Etching of N‐Doped Graphene Meshes as Metal‐Free Catalyst with Tunable Kinetics, High Activity and the Origin of New Catalytic Behaviors

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