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化学反应工程与工艺
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氮修饰载体负载Pd催化剂用于苯酚加氢制环己酮反应
1.中国石油化工股份有限公司上海石油化工研究院,绿色化工与工业催化国家重点实验室,上海 201208; 2.复旦大学化学系,上海 200433
Hydrogenation of Phenol to Cyclohexanone over Pd Catalysts Supported on Nitrogen-Modified Carrier
1. State Key Laboratory of Green Chemical Engineering and Industrial Catalysis, Shanghai Research Institute of Petrochemical Technology, SINOPEC, Shanghai 201208, China; 2. Department of Chemistry, Fudan University, Shanghai 200433, China
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摘要 苯酚加氢是一条较理想的环己酮制备路线,如何实现高转化率条件下目标产物的高选择性仍极具挑战。通过制备系列氮修饰载体,系统考察了Pd基催化体系中载体特性对苯酚加氢制环己酮反应的影响。结果表明:可通过在载体表面引入氮原子进行改性显著提高环己酮收率,且氮原子引入方式对反应结果影响显著。氮掺杂的纳米碳材料表现最佳,苯酚转化率达99.1%,同时环己酮选择性达到97.6%。载体CN-12中以结构修饰氮原子为主,氮原子进入骨架,形成类石墨相碳氮材料,更有利于增强载体表面的路易斯碱性,使得苯酚在载体表面形成“非共平面”吸附,有利于提高环己酮选择性。
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董 静1
刘 苏1
曹 勇2
刘永梅2
王仰东1
关键词 氮修饰载体Pd基催化剂苯酚环己酮催化加氢    
Abstract:Selective hydrogenation of phenol is an ideal process to produce cyclohexanone. However, to obtain high selectivity of cyclohexanone while obtaining high conversion of phenol has remained challenging. By preparing a series of nitrogen-modified carriers, the influence of the carrier characteristics in the Pd-based catalytic system on the hydrogenation of phenol to cyclohexanone was investigated systematically. It was found that the selectivity of cyclohexanone could be significantly improved by introducing nitrogen atoms on the surface of the carriers, and the nitrogen atom introducing mode had a significant influence on the reaction results. The nitrogen-doped nanocarbon materials showed the best performance, with phenol conversion up to 99.1% and cyclohexanone selectivity up to 97.6%. The carrier CN-12 mainly used structure-modified nitrogen atoms that entered into the skeleton to form graphite-like phase carbon and nitrogen materials, which was more conducive to enhancing the Lewis alkalinity on the surface of the carrier, making phenol form “non-co-plane” adsorption on the surface of the carrier to improve the selectivity of cyclohexanone.
Key wordsnitrogen-modified carrier    Pd-based catalysts    phenol    cyclohexanone    catalytic hydrogenation   
收稿日期: 2020-01-05     
作者简介: 董 静(1982—),女,高级工程师;王仰东(1967—),男,研究员,通讯联系人。E-mail: wangyd.sshy@sinopec.com。
引用本文:   
董 静1,刘 苏1,曹 勇2等. 氮修饰载体负载Pd催化剂用于苯酚加氢制环己酮反应[J]. 化学反应工程与工艺, 2020, 36(4): 314-318.
DONG Jing1,LIU Su1,CAO Yong2 et al. Hydrogenation of Phenol to Cyclohexanone over Pd Catalysts Supported on Nitrogen-Modified Carrier[J]. 化学反应工程与工艺, 2020, 36(4): 314-318.
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