Highly selective conversion of phenol to cyclohexanol over Ru/Nb2O5-nC18PA catalysts with increased acidity in a biphasic system under mild conditions

Zhan, Jiahui; Hu, Rui; Luo, Xin; Zhang, Cheng; Luo, Gang; Fan, Jiajun; Clark, James H.; Zhang, Shicheng

doi:10.1039/d1gc04046d

Cited by 32 publications

(11 citation statements)

References 70 publications

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“…According to the literature and the results obtained in this work, we proposed a plausible catalytic mechanism for the hydrogenation reaction catalyzed by PMS-22 (Scheme S1). 44 First, phenol was adsorbed on the surface of Ni 0 /nickel silicate heterojunction to combine with nickel silicate, which served as the Lewis acid site, and thus realized the activation of the aromatic ring. Meanwhile, the adjacent electron-deficient nickel site adsorbed, activated, and dissociated molecular H 2 into highly active H atoms, which would migrate and attack phenol on the neighboring nickel silicate.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

Stabilization of Ni⁰/Ni^II Heterojunctions inside Robust Porous Metal Silicate Materials for High-Performance Catalysis

Zhang

Shi

2022

Inorg. Chem.

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Heterostructural nanomaterials demonstrate great potential to replace noble metal-based catalysts because heterojunctions could induce relocalization of electrons and facilitate the migration of electrons and charge carriers at the heterostructural boundary between electron-rich and electrondeficient metal sites; however, the instability of heterojunctions greatly hinders their practical applications. We report herein an effective strategy for the fabrication and stabilization of Ni 0 /Ni II heterojunctions inside a porous metal silicate (PMS) material PMS-22 using a nickel coordination complex as the bifunctional template. The synergistic activity between metallic nickel and nickel silicate in PMS-22 highly boosts the catalytic activity in the hydrogenation of phenol, which could activate phenol at a very low temperature of 50 °C. Most importantly, PMS-22 demonstrates robust stability in catalysis, attributed to the strong interaction and charge transfer between metallic Ni and nickel silicate at the heterointerfaces inside the confined pores. Therefore, this work paves a new pathway to improve the stability and activity of heterostructural nanomaterials for catalytic applications.

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Section: ■ Results and Discussionmentioning

confidence: 99%

Stabilization of Ni⁰/Ni^II Heterojunctions inside Robust Porous Metal Silicate Materials for High-Performance Catalysis

Zhang

Shi

2022

Inorg. Chem.

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“…Cyclohexanol is the crucial intermediate for synthesizing nylon-66, caprolactam, and adipic acid in the petroleum industry 1,2 and is also a primary raw material for preparing surfactants, detergents, and plasticizers. 3 The main industrial production methods of cyclohexanol include cyclohexane oxidation, benzene hydrogenation, benzene−cyclohexene hydration, and phenol hydrogenation. However, cyclohexane oxidation has a low one-way yield, high energy consumption, and severe equipment corrosion.…”

Section: Introductionmentioning

confidence: 99%

Selective Hydrogenation of Phenolic Compounds to Cyclohexanols over Nanosheet Ni@Al₂O₃ Catalysts

Hao

Guo

Pan

et al. 2023

Ind. Eng. Chem. Res.

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Herein, a series of nanosheet Ni@Al 2 O 3 catalysts were prepared using the one-pot method, which offers good catalytic activity and selectivity of the phenolic compounds in aqueous due to their unique structures with rich active sites and large specific surface areas. The effects of calcination temperature, nickel loading, reaction temperature, and H 2 pressure on the catalyst's performance were studied on the simulated phenolic wastewater. The results indicated that phenolic compounds were selectively converted to the corresponding cyclohexanols regardless of the conversion by the 20%Ni@Al 2 O 3 -500 catalyst under mild conditions. Based on the procedure, cyclohexanol and water separation were simulated with the Aspen Plus model. This work provides an alternative scheme for treating phenolic wastewater.

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“…1,2 Furthermore, cyclohexanol can also be used as a solvent in pharmaceuticals, coatings, resins, etc. 3,4 At present, cyclohexanol is produced industrially through phenol hydrogenation and cyclohexane oxidation, while these methods have the disadvantages of high cost and being nonenvironmentally friendly. 5,6 Lignin is a renewable natural resource and has abundant reserves on earth.…”

Section: Introductionmentioning

confidence: 99%

“…Cyclohexanol, as a vital chemical raw material, has been widely applied in the production of hexamethylenediamine, adipic acid, and caprolactam. , Furthermore, cyclohexanol can also be used as a solvent in pharmaceuticals, coatings, resins, etc. , At present, cyclohexanol is produced industrially through phenol hydrogenation and cyclohexane oxidation, while these methods have the disadvantages of high cost and being non-environmentally friendly. , …”

Section: Introductionmentioning

confidence: 99%

Co-Based Catalysts Supported on Ceria with Different Shape Structures for Hydrodeoxygenation of Guaiacol

Wen

Zhao

et al. 2022

Energy Fuels

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CeO2 with three different morphologies of nanorods (CeO2-r), particles (CeO2-p), and cubes (CeO2-c) was prepared, and the guaiacol hydrodeoxygenation over their corresponding Co-based catalysts was performed at 160–220 °C, 2 MPa, a H2 flow rate of 80 mL/min, and a weight hourly space velocity of 0.7 h–1. Compared with Co/CeO2-p and Co/CeO2-c, Co/CeO2-r has smaller Co particle sizes, a higher Brunauer–Emmett–Teller surface area, and larger amount of Co active centers, oxygen vacancies, and weak acid sites. These better physicochemical properties for Co/CeO2-r provide more Co active sites for guaiacol hydrodeoxygenation, favor the adsorption and activation of guaiacol, and contribute to the cleavage of C–O. Therefore, Co/CeO2-r presents a maximum guaiacol conversion of 97.1% and the highest yield of cyclohexanol of 91.7% among these catalysts. The result shows that the shape structure of CeO2 has an important influence on the guaiacol hydrodeoxygenation performance over its corresponding catalysts.

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Highly selective conversion of phenol to cyclohexanol over Ru/Nb₂O₅-nC18PA catalysts with increased acidity in a biphasic system under mild conditions

Abstract: Cyclohexanol is an essential intermediate in the chemical industry for the synthesis of nylon and other materials, but the direct hydrogenation of phenol to produce cyclohexanol is problematic due to...

Cited by 32 publications

References 70 publications

Stabilization of Ni⁰/Ni^II Heterojunctions inside Robust Porous Metal Silicate Materials for High-Performance Catalysis

Stabilization of Ni⁰/Ni^II Heterojunctions inside Robust Porous Metal Silicate Materials for High-Performance Catalysis

Selective Hydrogenation of Phenolic Compounds to Cyclohexanols over Nanosheet Ni@Al₂O₃ Catalysts

Co-Based Catalysts Supported on Ceria with Different Shape Structures for Hydrodeoxygenation of Guaiacol

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Highly selective conversion of phenol to cyclohexanol over Ru/Nb2O5-nC18PA catalysts with increased acidity in a biphasic system under mild conditions

Abstract: Cyclohexanol is an essential intermediate in the chemical industry for the synthesis of nylon and other materials, but the direct hydrogenation of phenol to produce cyclohexanol is problematic due to...

Cited by 32 publications

References 70 publications

Stabilization of Ni0/NiII Heterojunctions inside Robust Porous Metal Silicate Materials for High-Performance Catalysis

Stabilization of Ni0/NiII Heterojunctions inside Robust Porous Metal Silicate Materials for High-Performance Catalysis

Selective Hydrogenation of Phenolic Compounds to Cyclohexanols over Nanosheet Ni@Al2O3 Catalysts

Co-Based Catalysts Supported on Ceria with Different Shape Structures for Hydrodeoxygenation of Guaiacol

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Highly selective conversion of phenol to cyclohexanol over Ru/Nb₂O₅-nC18PA catalysts with increased acidity in a biphasic system under mild conditions

Stabilization of Ni⁰/Ni^II Heterojunctions inside Robust Porous Metal Silicate Materials for High-Performance Catalysis

Stabilization of Ni⁰/Ni^II Heterojunctions inside Robust Porous Metal Silicate Materials for High-Performance Catalysis

Selective Hydrogenation of Phenolic Compounds to Cyclohexanols over Nanosheet Ni@Al₂O₃ Catalysts