Solvent-free aerobic oxidation of hydrocarbons and alcohols with Pd@N-doped carbon from glucose

Zhang, Pengfei; Gong, Yutong; Li, Haoran; Chen, Zhirong; Wang, Yong

doi:10.1038/ncomms2586

Cited by 342 publications

(166 citation statements)

References 59 publications

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“…It is immediately apparent that initial selox rates for the 0.74 wt% Pd/meso-Al 2 O 3 catalyst outperform those for the analogous amo -alumina support by at least a factor of two, and provides a 5 10 fold enhancement for crotyl and cinnamyl selox over mesoporous silica counterparts. Absolute rates scale inversely with molecular mass, decreasing in the order C 4 > C 5 ol > C 9 > C 10 > > C 15 as anticipated from the slower bulk and intra-pore diffusion (and greater steric constraints) of the bulkier alcohols [40]. For all substrates, the TOFs indicate a common form of active surface PdO is present over both alumina supports, but which differs from that present in the (less active) Pd/SBA-15 and Pd/KIT-6 catalysts.…”

Section: Allylic Alcohol Seloxmentioning

confidence: 99%

Selective oxidation of allylic alcohols over highly ordered Pd/meso-Al2O3 catalysts

Parlett

Durndell

Wilson

et al. 2014

Catalysis Communications

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Highly ordered mesoporous alumina was prepared via evaporation induced self-assembly and was impregnated to afford a family of Pd/meso-Al 2 O 3 catalysts for the aerobic selective oxidation (selox) of allylic alcohols under mild reaction conditions. CO chemisorption and XPS identify the presence of highly dispersed (0.9 2 nm) nanoparticles comprising heavily oxidised PdO surfaces, evidencing a strong palladium-alumina interaction. Surface PdO is confirmed as the catalytically active phase responsible for allylic alcohol selox, with initial rates for Pd/meso-Al 2 O 3 far exceeding those achievable for palladium over either amorphous alumina or mesoporous silica supports. Pd/meso-Al 2 O 3 is exceptionally active for the atom efficient selox of diverse allylic alcohols, with activity inversely proportional to alcohol mass.

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Section: Allylic Alcohol Seloxmentioning

confidence: 99%

Selective oxidation of allylic alcohols over highly ordered Pd/meso-Al2O3 catalysts

Parlett

Durndell

Wilson

et al. 2014

Catalysis Communications

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“…1,2 Utilization of O 2 or air as oxidizing agents to replace conventional stoichiometric d 0 -metal oxides is the final goal for environmentally benign oxidation reactions. To achieve this goal, tremendous efforts have been made to develop new catalysts, including monometallic Au, [3][4][5][6][7][8][9][10][11][12][13][14] Pd, [15][16][17][18] and bimetallic Au-Pd, [19][20][21][22][23][24][25][26][27] Au-Cu, 28, 29 Au-2 Ir 30 catalysts. Among them, Au-Pd catalysts usually show enhanced activity and selectivity in catalyzing alcohols to corresponding aldehydes or ketones compared to pure Au or Pd catalysts.…”

Section: Introductionmentioning

confidence: 99%

Theoretical Studies on the Synergetic Effects of Au–Pd Bimetallic Catalysts in the Selective Oxidation of Methanol

et al. 2015

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The selective oxidation of methanol to formaldehyde with molecular O 2 on Au-Pd alloy surfaces has been studied by using density functional theory (DFT). We show that the existence of Pd remarkably improves the adsorption and activation of O 2 on Au-Pd surfaces. In particular, the second-neighbor Pd monomer pair (Pd-SNMP) surrounded by gold atoms can provide unique active sites for the co-adsorption of O 2 …CH 3 OH, thus facilitating the activation of O 2 via a hydroperoxyl radical ( * OOH). With the involvement of * OOH and its decomposed fragments ( * O and * OH), the oxidative dehydrogenation of methanol to formaldehyde is facilely achieved on bimetallic Au-Pd surfaces, the barriers of which are calculated to be 0.02-0.45 eV on Au 2 Pd/(111) and AuPd/(100) surfaces.Importantly, we find that the unusual activation of O 2 via an OOH-pathway instead of direct dissociation on Au-Pd catalysts is mainly responsible for the enhanced activity and selectivity in the selective oxidation of alcohols. This hydroperoxyl-based mechanism reveals the intrinsic synergy of Au-Pd bimetallic catalysts in the selective oxidation of alcohols and may provide insights for designing better bimetallic catalysts.

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“…Carbon materials, including amorphous carbon, ordered mesoporous carbon, graphite/graphene (oxide) and carbon nanotubes, are widely applied in many catalytic transformations in modern organic chemistry [9][10][11] , and good performance has been obtained in the oxidation of an alkane [12][13][14][15] , alcohol [16][17][18] , amine 19 , thiol and sulphide 20,21 . These reactions encompass the oxidative hydrogen atom transfer reactions.…”

mentioning

confidence: 99%

Carbon-catalysed reductive hydrogen atom transfer reactions

et al. 2015

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Generally, transition metal catalysts are essential for the reductive hydrogen atom transfer reaction, which is also known as the transfer hydrogenation reaction or the borrowinghydrogen reaction. It has been reported that graphene can be an active catalyst in ethylene and nitrobenzene reductions, but no report has described carbon-based materials as catalysts for alcohol amination via the borrowing-hydrogen reaction mechanism. Here we show the results from the preparation, characterization and catalytic performance investigation of carbon catalysts in transition metal-free borrowing-hydrogen reactions using alcohol amination and nitro compound/ketone reduction as model reactions. XPS, XRD, SEM, FT-IR and N 2 adsorption-desorption studies revealed that C ¼ O group in the carbon catalysts may be a possible catalytically active site, and high surface area is important for gaining high activity. The activity of the carbon catalyst remained unchanged after reuse. This study provides an attractive and useful methodology for a wider range of applications.

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Solvent-free aerobic oxidation of hydrocarbons and alcohols with Pd@N-doped carbon from glucose

Cited by 342 publications

References 59 publications

Selective oxidation of allylic alcohols over highly ordered Pd/meso-Al2O3 catalysts

Selective oxidation of allylic alcohols over highly ordered Pd/meso-Al2O3 catalysts

Theoretical Studies on the Synergetic Effects of Au–Pd Bimetallic Catalysts in the Selective Oxidation of Methanol

Carbon-catalysed reductive hydrogen atom transfer reactions

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