Unveiling the active sites of graphene-catalyzed peroxymonosulfate activation

Duan, Xiaoguang; Sun, Hongqi; Ao, Zhimin; Zhou, Li; Wang, Guoxiu; Wang, Shaobin

doi:10.1016/j.carbon.2016.06.016

Cited by 390 publications

(156 citation statements)

References 42 publications

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“…Therefore, it was obvious that there was a remarkable synergistic effect in the EG/PDS combined system. This result was similar to the rGO/persulfate [16,32] or activated carbon /persulfate combined system studied by Zhang and Yang [45,46]. Therefore, it could be concluded that EG was also an excellent catalyst to activate persulfate decomposition and further induce the degradation of dye at an ambient temperature.…”

Section: Decolorization Of Ar97 In Different Systemssupporting

confidence: 85%

“…Second, the EG was sufficiently annealed at a high temperature, and the structure has been improved [39]. It was worth noting that the I D /I G value of EG was much lower than that of graphene (I D /I G > 1) [32], sulfur-doped hierarchically porous carbon (~1) [25], and mesoporous carbon (1.2) [40].…”

Section: Materials Characterizationmentioning

confidence: 99%

“…Sun et al [16] first reported that reduced graphene oxide prepared by a hydrothermal method demonstrated an excellent catalytic ability to activate PMS for pollutant oxidation. Graphene oxide, graphitic oxide [29][30][31], and reduced graphene oxide [32] were often prepared by Hummers or a modified Hummers method, which needed a lot of oxidant (mass potassium permanganate /mass natural graphite ≈ 3/1), strict temperature conditions (e.g., ice bath and so on), and other complicated process and reagents. Compared with GO and rGO, the preparation of EG needed less oxidant, and the method was much simpler (as shown in Section 3.2.…”

Section: Introductionmentioning

confidence: 99%

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Preparation and Catalytic Performance of Expanded Graphite for Oxidation of Organic Pollutant

Lan

2019

Catalysts

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A classic carbon material—expanded graphite (EG), was prepared and proposed for a new application as catalysts for activating peroxydisulfate (PDS). EG samples prepared at different expansion temperatures were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and other methods. It was observed that there existed a remarkable synergistic effect in the EG/PDS combined system to degrade Acid Red 97 (AR97). Unlike other carbon material catalysts, sp2 carbon structure may be the main active site in the catalytic reaction. The EG sample treated at 600 °C demonstrated the best catalytic activity for the activation of PDS. Degradation efficiency of AR97 increased with raising PDS dosage and EG loadings. The pH of aqueous solution played an important role in degradation and adsorption, and near-neutrality was the optimal pH in this research. It was assumed that the radical pathway played a dominant role in AR97 degradation and that oxidation of AR97 occurred in the pores and interface layer on the external surface of EG by SO4·− and ·OH, generated on or near the surface of EG. The radical oxidation mechanism was further confirmed by electron paramagnetic resonance spectroscopy. The EG sample could be regenerated by annealing, and the catalytic ability was almost fully recovered.

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Section: Decolorization Of Ar97 In Different Systemssupporting

confidence: 85%

Section: Materials Characterizationmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Preparation and Catalytic Performance of Expanded Graphite for Oxidation of Organic Pollutant

Lan

2019

Catalysts

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“…Acetone was used to mimic the inactive sites, the linear chain aliphatic ketone (C sp3 =O). Such modeling has been widely employed to afford a favorable compromise between precision and computational effort ,, . Scheme a–c illustrates the variation of O 2 interacting with these models and the corresponding adsorption barrier energies (Eads).…”

Section: Resultsmentioning

confidence: 99%

Carbon Catalyzed Hydroxylation of Benzene with Dioxygen to Phenol over Surface Carbonyl Groups

Shan

Cai

et al. 2019

ChemCatChem

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Carbon materials are promising environmentally-benign heterogeneous catalysts but design of effective carbon catalysts with comparable or even superior performance to metal-based ones is highly challengeable. Herein, N-doped mesoporous carbons with the surface enriched with abundant oxygen species were synthesized by a facile hydrothermal doping strategy in the self-assembly of phenolic resin, followed with a carbonization process. Direct hydroxylation of benzene to phenol with O 2 as the sole oxidant was effectively catalyzed by these carbons, affording a yield superior or comparable to previous efficient transition metal and even noble metal-based catalysts. The catalyst is facilely recovered and stably reused. The surface carbonyl groups are the active sites for O 2 activation (rate determining step) to generate hydroxyl radicals, which are the reactive oxygen species to oxidize the benzene. This methodology is readily extendable to the oxidation of various other benzene derivatives.[a] W.

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“…Through the above systematic studies, af acile and efficient methodt os electively modify the surface of CNTsa nd generate active oxygen functionalities was successfully developed. As schematically depicted in Figure 3, the magnesium nitrate salts decompose, and the surfacec arbona toms can be removed by NO 2 to generate defects such as surface vacancies in the carbon matrixo re dged sites of the graphene layer.S everal studies reported that these skeleton defects wereb eneficial to the selectivei ntroduction of ketonic carbonyl groups in the presence of oxygen, [17,19] and the increase of quinone functionalities on the carbon-based materialp romoted the selective dehydrogenation. [5a] The main idea behind the modification of CNTsw ith magnesium nitrate salts was to create defects prone to be oxidizedinsitu into quinone groups, which are beneficial for the ODH of n-butane to butenes and butadiene.…”

mentioning

confidence: 99%

A Facile and Efficient Method to Fabricate Highly Selective Nanocarbon Catalysts for Oxidative Dehydrogenation

et al. 2016

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Carbon nanotubes (CNTs) were used in oxidative dehydrogenation (ODH) reactions. Quinone groups on the CNT surface were identified as active sites for the dehydrogenation pathway. Liquid-phase oxidation with HNO is one way to generate various oxygen functionalities on the CNT surface but it produces a large amount of acid waste, limiting its industrial application. Here, a facile and efficient oxidative method to prepare highly selective CNT catalysts for ODH of n-butane is reported. Magnesium nitrate salts as precursors were used to produce defect-rich CNTs through solid-phase oxidation. Skeleton defects induced on the CNT surface resulted in the selective formation of quinone groups active for the selective dehydrogenation. The as-prepared catalyst exhibited a considerable selectivity (58 %) to C olefins, which is superior to that of CNTs oxidized with liquid HNO . Through the introduction of MgO nanoparticles on the CNT surface, the desorption of alkenes can be accelerated dramatically, thus enhancing the selectivity. This study provides an attractive way to develop new nanocarbon catalysts.

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Unveiling the active sites of graphene-catalyzed peroxymonosulfate activation

Cited by 390 publications

References 42 publications

Preparation and Catalytic Performance of Expanded Graphite for Oxidation of Organic Pollutant

Preparation and Catalytic Performance of Expanded Graphite for Oxidation of Organic Pollutant

Carbon Catalyzed Hydroxylation of Benzene with Dioxygen to Phenol over Surface Carbonyl Groups

A Facile and Efficient Method to Fabricate Highly Selective Nanocarbon Catalysts for Oxidative Dehydrogenation

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