Preparation of Defective Niobium-Based Catalysts to Address the “Seesaw Effect” in Phenol Hydrodeoxygenation

IF 7.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Shilong Liu, Gege Pan, MiaoMiao Wei, Baoyan Zhi, Yanchang Zhang, Chengjun Hu, Hao Li
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Abstract

Cyclohexanone, a product of phenol hydrogenation, is a very reactive intermediate, which can easily generate byproducts such as cyclohexanol and cyclohexane, and there is a difficult-to-regulate “seesaw effect”. In this paper, a defective catalyst, Pd/Nb2O5-800-AP, was synthesized by the hydrothermal method at 170 °C and 1 MPa H2, aiming to break the difficult equilibrium between the high conversion of phenol and the high selectivity of cyclohexanone, which has a good industrial prospect. By changing the calcination temperature of the carrier to control the surface defect content, Pd was placed in an electron-rich state, which promoted the activation of hydrogen molecules and adsorption of phenol in a “nonplanar” manner, which was favorable for the generation of cyclohexanone as a product. In addition, the formation of electron-deficient oxygen defects and low-valent Nb4+ on the surface of the AP-treated catalysts promoted the adsorption and activation of oxygen-containing functional groups, which enhanced the activity of the phenol HDO reaction.

Abstract Image

制备缺陷铌基催化剂解决苯酚加氢脱氧过程中的“跷跷板效应”
环己酮是苯酚加氢的产物,是一种反应性很强的中间体,很容易生成环己醇、环己烷等副产物,存在难以调节的“跷跷板效应”。本文在170℃、1 MPa H2条件下,采用水热法合成了一种缺陷催化剂Pd/Nb2O5-800-AP,旨在打破苯酚高转化率与环己酮高选择性之间的难平衡,具有良好的工业前景。通过改变载体的煅烧温度来控制表面缺陷含量,将Pd置于富电子状态,促进氢分子的活化和苯酚的“非平面”吸附,有利于生成环己酮作为产物。此外,经过ap处理的催化剂表面形成缺电子氧缺陷和低价Nb4+,促进了含氧官能团的吸附和活化,从而增强了苯酚HDO反应的活性。
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来源期刊
ACS Sustainable Chemistry & Engineering
ACS Sustainable Chemistry & Engineering CHEMISTRY, MULTIDISCIPLINARY-ENGINEERING, CHEMICAL
CiteScore
13.80
自引率
4.80%
发文量
1470
审稿时长
1.7 months
期刊介绍: ACS Sustainable Chemistry & Engineering is a prestigious weekly peer-reviewed scientific journal published by the American Chemical Society. Dedicated to advancing the principles of green chemistry and green engineering, it covers a wide array of research topics including green chemistry, green engineering, biomass, alternative energy, and life cycle assessment. The journal welcomes submissions in various formats, including Letters, Articles, Features, and Perspectives (Reviews), that address the challenges of sustainability in the chemical enterprise and contribute to the advancement of sustainable practices. Join us in shaping the future of sustainable chemistry and engineering.
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