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Facile synthesis of nitrogen-doped graphene via low-temperature pyrolysis: The effects of precursors and annealing ambience on metal-free catalytic oxidation

TLDR
In this article, a green and facile protocol of thermal treatment of graphene oxide (GO) with urea was adopted to synthesize nitrogen-doped graphene (NG-Urea-air) at a low temperature (350°C) in the static air.
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This article is published in Carbon.The article was published on 2017-05-01 and is currently open access. It has received 299 citations till now. The article focuses on the topics: Graphene & Carbocatalysis.

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Current state of green reduction strategies: Solution-processed reduced graphene oxide for healthcare biodetection.

TL;DR: The degrees of gaining tips with the solution-based green reduction methods, conditions, complexity and the resulting rGO characteristics have been elucidated comparatively and the characterization scheme for graphene-based materials are outlined for the future endeavours.
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Activation of peroxymonosulfate by WTRs-based iron-carbon composites for atrazine removal: Performance evaluation, mechanism insight and byproduct analysis

TL;DR: In this paper, water treatment residuals (WTRs) were calcinated to synthesize iron carbon composites, which were then applied to activate peroxymonosulfate (PMS) for the elimination of herbicide atrazine.
Journal ArticleDOI

Role of different dimensional carbon nanoparticles in catalytic oxidation of organic pollutants and alleviating membrane fouling during ultrafiltration of surface water

TL;DR: In this paper, carbon nanoparticles in different structural dimensions, including carbon nanotubes (CNTs), carbon nanofibers (CNFs), hexagonally (CMK-3) and cubically ordered mesoporous carbons were proposed for peroxymonosulfate (PMS) activation.
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Modulation of carbon induced persulfate activation by nitrogen dopants: recent advances and perspectives

TL;DR: In this article, a review of nitrogen-doped carbon catalysts in advanced oxidation processes based on persulfates (PS-AOPs) is presented, where the relationships between structure and activity are particularly focused and comprehensively discussed through statistical analysis.
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The use of industrial molasses waste in the performant synthesis of few-layer graphene (and its Au/Ag nanoparticles nanocomposites): Photocatalytic and supercapacitance applications

TL;DR: In this paper , a green, simple, easily scalable, fast, and highly efficient synthesis of few-layer graphene and its composites with Au and Ag nanoparticles using a waste is presented.
References
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Journal ArticleDOI

Electric Field Effect in Atomically Thin Carbon Films

TL;DR: Monocrystalline graphitic films are found to be a two-dimensional semimetal with a tiny overlap between valence and conductance bands and they exhibit a strong ambipolar electric field effect.
Journal ArticleDOI

The rise of graphene

TL;DR: Owing to its unusual electronic spectrum, graphene has led to the emergence of a new paradigm of 'relativistic' condensed-matter physics, where quantum relativistic phenomena can now be mimicked and tested in table-top experiments.
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Raman spectrum of graphene and graphene layers.

TL;DR: This work shows that graphene's electronic structure is captured in its Raman spectrum that clearly evolves with the number of layers, and allows unambiguous, high-throughput, nondestructive identification of graphene layers, which is critically lacking in this emerging research area.
Journal ArticleDOI

Synthesis of graphene-based nanosheets via chemical reduction of exfoliated graphite oxide

TL;DR: In this paper, a colloidal suspension of exfoliated graphene oxide sheets in water with hydrazine hydrate results in their aggregation and subsequent formation of a high surface area carbon material which consists of thin graphene-based sheets.
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Frequently Asked Questions (19)
Q1. What are the contributions in "Facile synthesis of nitrogen-doped graphene via low-temperature pyrolysis: the effects of precursors and annealing ambience on metal-free catalytic oxidation" ?

In this paper, the authors applied a facile strategy by direct treatment of GO and urea at a moderate temperature ( 350 °C ). 

The annealing process with a slowheating rate (5 °C/min) also effectively inhibited the polycondensation of urea as the process only occurs during the rapidly thermal polymerization in the presence of large amounts of urea. 

the acidic/basic condition of the reaction solutions can impact the catalytic performance of metal catalysts as the strong acidic condition can destroy the metal crystalline structure and lead to severe metal leaching. 

Introducing heteroatoms (B, N, O, P, S, and so forth) into the carbon lattice can effectively disorientate the homogeneously conjugated electron network and modulate the surface properties by tweaking the charge distribution and spinning culture of the doped domains [13, 14]. 

Their pioneering studies integrating with material design and theoretical calculations revealed that, due to a greater electronegativity (χN = 3.04) compared with the carbon atom (χC = 2.55), N-doping can effectivtly interrupt the highly-conjugated carbon network of graphene and induce the electron transport from the neighbouring carbon to nitrogen atoms, giving rise to positively charged carbon atoms [37, 38]. 

Many studies have reported that N-doping can effectively break the inertness of sp2 hybridized carbon lattice and dramatically tailor the electron density and spin culture of the adjacent carbon, giving rise to the superb catalytic performances in electrochemistry, hydrocarbon conversion, and superoxide activation [34-36]. 

Their previous study also indicated raising the annealing temperature in inert atmosphere would result in a lower N-doping level due to the breakup of C-N bond while affording a higher proportion of quaternary N benefiting from the better thermal stability of graphitic N, which is simultaneously bonded with three carbon atoms with substitutional doping in the carbon framework [26]. 

The mild annealing and doping processes favored the oxidative atmosphere due to the induced structure defects such as edging sites and vacancies which enabled carbon reconstruction for N-doping. 

the rGO can be used as a better carbon precursor to prepare nitrogen-doped graphene with a desirable SSA, N-doping level, defective degree, and stunning catalytic activity. 

With respect to rGO, the re-constructing of graphene boundaries (edging sites) and lattice during annealing may also help attain certain amounts of N-doping as shown in this study. 

The green and efficient carbocatalysts have demonstrated extraordinary potentials for activating various superoxides (e.g. peroxymonosulfate, persulfate, hydrogen peroxide, and ozone) for the oxidative removal of toxic pollutants in wastewater without any secondary contamination [18-21]. 

Both organic substances and inorganic salts were applied as the nitrogen precursors for nitrogen doping and urea was discovered to be the best precursor with a high doping level and better reducibility without any polycondensation. 

The experimental results indicated that the nitrogen-doped graphene with a higher proportion of graphitic N at a similar doping level exhibited a better catalytic activity for phenol oxidation, and the densities functional theory (DFT) calculations further evidenced that the adsorption of PMS molecules at the adjacent carbon of graphitic N exhibited the lowest adsorption energy and greatest tendency for electron transfer from carbon lattice to PMS for the activation of superoxide O-O bond [26]. 

The proportion of graphitic N of NG-Urea-air and N-rGO-air in total nitrogen was low due to the fact that the mild annealing temperature cannot produce high contents of substitutional N-doping into the carbon lattice. 

The outstanding efficiency of PMS activation on nitrogen-doped graphene is also contributed by the non-radical process, in which the PMS molecules are activated at N-doped domains and followed by readily oxidation of target organics via electron transfer as illustrated in Fig. 

due to the complicated structure and surface chemistry of nanocarbons, the mechanism of carbocatalysis in metal-free oxidation remains ambiguous, leaving more blanks for mechanisticstudy. 

Fig. S8 manifested that the phenol oxidation rate was speeded up with the increased nitrogen amount in graphene, suggesting that the high doping level leads to a promoted catalytic performance for PMS activation. 

The ammonium salts would decompose during the thermal annealing and release NH3 (the doping agent) and other gasses (N2, N2O, or HCl), which facilitate the formation of porous N-doped graphene with larger SSAs, pore size, and pore volume (Fig. S9 and Table S2). 

The XPS surveys in Fig. 3a illustrate that thermal annealing effectively eliminated the oxygen groups of the graphene oxide (31.4 at.%, Table 1) to form a more reductive surface of rGO-air (14.3 at.%).