Modular calcination strategy to construct defect-rich nitrogen-doped Nb2O5 for boosting photocatalytic oxidation of cyclohexane to cyclohexanone in solvent-free conditions

煅烧 环己烷 环己酮 光催化 溶剂 兴奋剂 化学 无机化学 氮氧化物 光化学 材料科学 化学工程 有机化学 催化作用 燃烧 工程类 光电子学
作者
Kuan Wang,Dan Wang,Xiaoyong Zhang,Junlei Wang,Shengli Lv,Zhen‐Hong He,Huan Wang,Weitao Wang,Yang Yang,Zhao‐Tie Liu
出处
期刊:Applied Surface Science [Elsevier BV]
卷期号:617: 156600-156600 被引量:12
标识
DOI:10.1016/j.apsusc.2023.156600
摘要

The partial oxidation of cyclohexane (CHA) with oxygen to cyclohexanone (CHA-one) is one of the most transformation in the chemical industry in view that CHA-one is an irreplaceable raw material in the production of nylon. Herein, hydrogen, vacuum and air modules combined with ammonia module, respectively, were used to construct defect-rich nitrogen-doped Nb2O5. And, the calcination order and temperature were also considered to establish a modular calcination strategy. A series of modified N-doped Nb2O5 were prepared by the proposed strategy, which were used to catalyze the photo-oxidation of CHA in solvent-free and room temperature conditions. Among these modified N-doped Nb2O5 samples, the HN-Nb2O5 possessed abundant chemical defects of oxygen vacancies and Nb4+, and achieved the best photocatalytic performance. Surprisingly, HN-Nb2O5 achieved an amount of 130.35 μmol for CHA-one, which was approximately 2.2 and 26 times that of the pure Nb2O5 and commercial Nb2O5, respectively, with up to 96.68% selectivity to CHA-one. The outstanding photocatalytic performance of the HN-Nb2O5 can be ascribed to the presence of chemical defect-rich and the NOx species, enhanced light absorption and effective electron-hole separation. DFT calculations explained the promotion of the chemical defects and N doping on Nb2O5 photocatalytic activity in terms of the band electron and band-gap level. The results of EPR analysis and scavenger tests found that e− is the main active species resulted in photocatalytic activity, while O2− is the dominant active species for producing CHA-one in the photo-oxidation of CHA. The present work developed an efficient strategy to construct the defect-rich N-doped metal oxide for the improved photocatalytic oxidation of hydrocarbon.
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