Studies of synergy between metal–support interfaces and selective hydrogenation of HMF to DMF in water

Goyal, Reena; Sarkar, Bipul; Bag, Arijit; Siddiqui, Nazia; Dumbre, Deepa K.; Lucas, Nishita; Bhargava, Suresh K.; Bordoloi, Ankur

doi:10.1016/j.jcat.2016.05.012

Cited by 108 publications

(95 citation statements)

References 57 publications

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“…Figure a shows the small‐angle X‐ray scattering patterns of the mesoporous carbon materials with different ratios of silver and tungsten. All samples show a sharp peak at a low angle with two higher‐order peaks, which can be assigned to the (100), (110), and (200) planes of the hexagonal space group p 6 mm . The intensity of the peaks is less compared to the hard template AgW‐SiO 2 (Figure S1 in the Supporting Information).…”

Section: Resultsmentioning

confidence: 99%

“…Whereas the other two peaks at 286.5 and 288.5 eV indicate the presence of oxygen functionalities at the surface, such as CO or C=O groups. The N 1s spectrum was also deconvoluted into three peaks; the peaks at 398.9, 400.1, and 403.5 eV are related to the presence of N‐pyridine, N‐pyrrolic, and N‐quaternary structures of the AgWCN x ‐1catalyst, respectively …”

Section: Resultsmentioning

confidence: 99%

“…The concept of metal nanoparticles supported on carbon materials has gained much attention. The homogeneous immobilization of different transition‐metal nanoparticles on mesoporous carbon nitride (CN x ) materials not only favors metal–support interactions but also enhances the capability of the catalyst for industrial application . In our previous report, we have shown the importance of the immobilization of WO x nanoclusters on MCN x for an acid–base co‐operative catalysis .…”

Section: Introductionmentioning

confidence: 99%

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Synthesis of AgWCN_x Nanocomposites for the One‐Step Conversion of Cyclohexene to Adipic Acid and Its Mechanistic Studies

Goyal

Sameer

Sarkar

et al. 2017

Chemistry A European J

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A novel catalyst composed of silver nanoparticles grafted on WCN has been prepared by using a facile pH-adjusted method. The material reported in this study presents a non-mineral acid route for the synthesis of the industrially significant monomer adipic acid through the selective oxidation of cyclohexene. Ag has been stabilized in the hydrophobic matrix during the formation of the mesoporous silica material by using aniline as stabilizing agent. A cyclohexene conversion of 92.2 % with 96.2 % selectivity for adipic acid was observed with the AgWCN -2 catalyst, therefore, the AgWCN catalyst was found to be efficient for the direct conversion to adipic acid with respect to their monometallic counterparts. The energy profile diagrams for each reaction path by using the AgWCN catalyst were studied along with their monometallic counterparts by using the Gaussian 09 package. The reported material can avoid the use of harmful phase-transfer catalysts (PTC) and/or chlorinated additives, which are two among other benefits of the reported work.

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Synthesis of AgWCN_x Nanocomposites for the One‐Step Conversion of Cyclohexene to Adipic Acid and Its Mechanistic Studies

Goyal

Sameer

Sarkar

et al. 2017

Chemistry A European J

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“…Thus, O 2 is initially placed on the Au atom at the apex site with side‐on coordination (Figure b). This active site was also confirmed by using the condensed Fukui function as presented in Table S6 and Table S7 (in the Supporting Information). Upon adsorption, the distances between Au NC and O 2 , namely, Au1−O1 and Au2−O2 are 2.35 Å and 2.39 Å, respectively.…”

Section: Resultsmentioning

confidence: 99%

Intramolecular Hydroamination by a Primary Amine of an Unactivated Alkene on Gold Nanoclusters: A DFT Study

2017

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Density functional theory calculations have been used to investigate the mechanism of intramolecular hydroamination of unactivated alkenes by using primary amines on gold nanoclusters (NCs) under aerobic conditions. By examining the activation modes in the cyclization process, the olefin activation mechanism was calculated to be the most energetically feasible of the three possible pathways. The amine activation pathway suffered from a high activation barrier, which means that this pathway is unlikely to take place on gold NCs. The catalytic cycle comprises five elementary steps: (1) adsorption of O2 on Au NCs results in superoxo‐like species and provides Lewis acidic sites that allow the nucleophilic substrate, 2,2‐diphenyl‐4‐penten‐1‐amine, to be adsorbed effectively; (2) intramolecular cyclization (C−N bond formation) takes place on the Au NCs through anti‐addition of the amino group; (3) hydroperoxy moiety formation by hydrogen transfer from the cyclic intermediate to superoxo‐like species; (4) the formation of hydrogen peroxide and (5) product involves hydrogen transfer from a hydrated formic acid. Natural bond orbital analysis of the transition states that arise during C−N bond formation reveals that anti‐addition of the substrate is preferred over the syn‐addition mechanism. A possible side reaction, the formation of 2‐methylene‐4,4‐diphenylpyrrolidine through β‐hydrogen elimination, is also discussed.

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“…In order to explore the graphitic like CNx structure, a series of Raman spectra of the CNx materials carbonized at different temperature has been carried out, and the results was shown in Figure d. All the CNx materials shows two distinct Raman band; graphitic band (G‐band) near 1590 cm −1 and distorted band (D‐band) near 1350 cm −1 ,. Interestingly, with the increase in carbonization temperature D‐band shift from 1591 to 1610 cm −1 with loss of peak intensity (in Figure d).…”

Section: Figurementioning

confidence: 99%

Role of Pyridinic Nitrogen on Base Catalyzed Knoevenagel Condensation over Pristine CNx

et al. 2017

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On a special focus, we have fabricated N2 doped mesoporous ordered CNx material using hexagonal SBA‐15 as hard template through polymerisation of hexamethylene tetramine precurssor. The synthesised materials exhibit a very high specific surface area 1332 cm3/g and pore volume 1.12 cc/g. The HR‐TEM shows the succesful replication of silica template i.e, tubular structure of material. The catlytic activity of material has been tested for Knoevenagel condensation reaction of benzaldehyde and ethyl cyanoacetate. Almost 93 % conversion of benzaldehyde has been achieved within 20 min of reaction at room temperature with ≥99.9 % product selectivity.

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Studies of synergy between metal–support interfaces and selective hydrogenation of HMF to DMF in water

Cited by 108 publications

References 57 publications

Synthesis of AgWCN_x Nanocomposites for the One‐Step Conversion of Cyclohexene to Adipic Acid and Its Mechanistic Studies

Synthesis of AgWCN_x Nanocomposites for the One‐Step Conversion of Cyclohexene to Adipic Acid and Its Mechanistic Studies

Intramolecular Hydroamination by a Primary Amine of an Unactivated Alkene on Gold Nanoclusters: A DFT Study

Role of Pyridinic Nitrogen on Base Catalyzed Knoevenagel Condensation over Pristine CNx

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Studies of synergy between metal–support interfaces and selective hydrogenation of HMF to DMF in water

Cited by 108 publications

References 57 publications

Synthesis of AgWCNx Nanocomposites for the One‐Step Conversion of Cyclohexene to Adipic Acid and Its Mechanistic Studies

Synthesis of AgWCNx Nanocomposites for the One‐Step Conversion of Cyclohexene to Adipic Acid and Its Mechanistic Studies

Intramolecular Hydroamination by a Primary Amine of an Unactivated Alkene on Gold Nanoclusters: A DFT Study

Role of Pyridinic Nitrogen on Base Catalyzed Knoevenagel Condensation over Pristine CNx

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Synthesis of AgWCN_x Nanocomposites for the One‐Step Conversion of Cyclohexene to Adipic Acid and Its Mechanistic Studies

Synthesis of AgWCN_x Nanocomposites for the One‐Step Conversion of Cyclohexene to Adipic Acid and Its Mechanistic Studies