Controllable Synthesis of 1D Pd@N-CNFs with High Catalytic Performance for Phenol Hydrogenation
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Controllable Synthesis of 1D Pd@N‑CNFs with High Catalytic Performance for Phenol Hydrogenation Chunhua Zhang1,2 · Jiuxuan Zhang1 · Yanhua Shao1 · Hong Jiang1 · Rizhi Chen1 · Weihong Xing1 Received: 17 June 2020 / Accepted: 28 August 2020 © Springer Science+Business Media, LLC, part of Springer Nature 2020
Abstract Achieving both high conversion and selectivity under mild conditions still remains a big challenge in the selective hydrogenation of phenol to cyclohexanone. Herein, one-dimensional (1D) N-doped carbon nanofibers (N-CNFs) were successfully fabricated by electrospinning with one-step carbonization, and used to load Pd nanoparticles for synthesizing Pd@N-CNFs catalysts. The dicyandiamide (DICY) and citric acid in the spinning solution exhibited a significant synergistic effect in controlling the morphology and surface property of N-CNFs and the corresponding catalytic activity of Pd@N-CNFs in the selective hydrogenation of phenol to cyclohexanone. The as-prepared [email protected] catalyst possessed good fibrous morphology, larger surface area, and more amounts of surface N and OH group, and exhibited a phenol conversion of 99.7% with a cyclohexanone selectivity of 97.3% under mild reaction conditions. In addition, the catalytic activity of [email protected] increased by 2.75 times as compared to Pd@N-CNFs-0 and 1.22 times in comparison with Pd@N-CNFs-100. Furthermore, the 1D [email protected] was easy to be recovered from the reaction mixture, and showed good reusability. Graphic Abstract
The proper molar ratio of dicyandiamide (DICY) and citric acid could significantly adjust the fibrous characteristic and surface properties of the Pd@CNFs catalyst, which contributed to the higher N and OH group contents, thereby improving Electronic supplementary material The online version of this article (https://doi.org/10.1007/s10562-020-03374-x) contains supplementary material, which is available to authorized users. Extended author information available on the last page of the article
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the loading and distribution of Pd nanoparticles and the dispersibility of Pd@CNFs in water. These properties jointly led to the superior phenol hydrogenation efficiency of the Pd@CNFs catalyst. Keywords N-doped carbon nanofibers · Electrospinning · Synergistic effect · Phenol hydrogenation · Cyclohexanone
1 Introduction Cyclohexanone is an important organic intermediate, and mainly used as the feedstock for synthesizing caprolactam and adipic acid, the intermediates for manufacturing Nylon-6 and Nylon-66, respectively [1, 2]. Industrially, the conventional production process of cyclohexanone is the oxidation of cyclohexane or hydrogenation of phenol. Cyclohexane oxidation not only requires high temperature and pressure but also produces undesirable byproducts and leads to low cyclohexanone selectivity [3]. For phenol hydrogenation, cyclohexanone is usually produced through one-step or two-step process. The two-step process contains phenol hydrogenation to cyclohexanol and subsequent cyclohe
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