Direct catalytic hydroxylation of benzene to phenol catalyzed by vanadia supported on exfoliated graphitic carbon nitride

Ionic liquids (ILs) have the advantages of low cost, eco-friendliness, abundant heteroatoms, excellent solubility, and coordinated ability with metal ions. These features make ILs a suitable precursor for fabricating metal singleatom catalysts (SACs). Herein, we prepared various metal single atoms anchored on ultrathin N-doped nanosheets (denoted as Cu 1 /NC, Fe 1 /NC, Co 1 /NC, Ni 1 /NC, and Pd 1 /NC) by direct pyrolysis using ILs and g-C 3 N 4 nanosheets as templates. Taking benzene oxidation to phenol with H 2 O 2 as a model reaction to evaluate their catalytic performance and potential applications, Cu 1 /NC calcined at 1000°C (denoted as Cu 1 /NC-1000) exhibits the highest activity with a turnover frequency of about 200 h −1 in the first 1 h at 60°C , which is better than that of most metal SACs reported in the literature. High benzene conversion of 82% with high phenol selectivity of 96% and excellent recyclability were achieved using the Cu 1 /NC-1000 catalyst. This study provides an efficient general strategy for fabricating SACs using ILs for catalytic applications.

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“…SCIENCE CHINA Materials model reaction to evaluate the catalytic performance of the asprepared metal SACs [46]. As shown in Fig.…”

Section: Articlesmentioning

confidence: 99%

Ionic-liquid-assisted synthesis of metal single-atom catalysts for benzene oxidation to phenol

Shen

Chen

et al. 2021

Sci. China Mater.

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“…Nitrogen-doped carbon materials have been found to be active for hydroxylation of benzene with H 2 O 2 under mild condition yet shows low catalytic activity (Yang et al., 2013). Metal-doped carbon nitride shows an improved activity for hydroxylation of benzene with H 2 O 2 to phenol but still remains unsatisfactory (Chen et al., 2009, Di et al., 2010, Xu et al., 2018, Zhang et al., 2018a, Zhang et al., 2018b; Hosseini et al., 2018). Therefore, developing efficient catalysts for benzene hydroxylation with H 2 O 2 to phenol is of great urgency.…”

Section: Introductionmentioning

confidence: 99%

Single Atomic Cu-N2 Catalytic Sites for Highly Active and Selective Hydroxylation of Benzene to Phenol

Zhang

Nie

et al. 2019

iScience

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Searching for an efficient single-atom catalyst for benzene hydroxylation to phenol is of critical importance, but it still remains a challenge. Herein, a single-atom catalyst with unique Cu-N 2 moieties (Cu 1-N 2 /HCNS) was prepared and confirmed by HAADF-STEM and EXAFS. Turnover number (TON) over Cu 1-N 2 /HCNS (6,935) is 3.4 times of Cu 1-N 3 /HCNS (2,034) under the same reaction conditions, and both exhibit much higher phenol selectivity (close to 99%) and stability compared with Cu nanoparticles and nanoclusters. Experiments and DFT calculations reveal that atomically dispersed Cu species are active sites for benzene hydroxylation to phenol, and the Cu-N 2 is more active than Cu-N 3 owing to its much lower energy barrier concerning the activation of H 2 O 2 led by its unique coordination state of local atomic structure. We envision that this work opens a new window for modulating coordination environments of single metallic atoms in catalysis design.

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“…This preparation demanded a silica-etching procedure with a volatile and toxic HF or NH4HF2 solution, which was time-consuming and not environmentally friendly [15,27,28]. To circumvent these issues we, very recently, developed vanadia catalysts supported on exfoliated g-C3N4 nanosheets, which were more conveniently synthesized than mesoporous g-C3N4 [29]. However, the final catalytic activity of such catalysts in the hydroxylation of benzene is still not satisfactory.…”

Section: Introductionmentioning

confidence: 99%

Facile synthesis of Fe-containing graphitic carbon nitride materials and their catalytic application in direct hydroxylation of benzene to phenol

Xue

Chen

Yin

et al. 2018

Chinese Journal of Catalysis

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Direct catalytic hydroxylation of benzene to phenol catalyzed by vanadia supported on exfoliated graphitic carbon nitride

Cited by 43 publications

References 55 publications

Ionic-liquid-assisted synthesis of metal single-atom catalysts for benzene oxidation to phenol

Ionic-liquid-assisted synthesis of metal single-atom catalysts for benzene oxidation to phenol

Single Atomic Cu-N2 Catalytic Sites for Highly Active and Selective Hydroxylation of Benzene to Phenol

Facile synthesis of Fe-containing graphitic carbon nitride materials and their catalytic application in direct hydroxylation of benzene to phenol

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