物理化学学报 >> 2016, Vol. 32 >> Issue (10): 2574-2580.doi: 10.3866/PKU.WHXB201606294

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B-TS-1分子筛的合成及其催化氧化性能

王磊,尹寒梅,王健豪,吴立志,刘月明*()   

  • 收稿日期:2016-05-03 发布日期:2016-09-30
  • 通讯作者: 刘月明 E-mail:ymliu@chem.ecnu.edu.cn
  • 基金资助:
    国家自然科学基金(U1462106);上海市重点学科建设项目基金(B409)

Synthesis and Catalytic Oxidation Performance of B-TS-1

Lei WANG,Han-Mei YIN,Jian-Hao WANG,Li-Zhi WU,Yue-Ming LIU*()   

  • Received:2016-05-03 Published:2016-09-30
  • Contact: Yue-Ming LIU E-mail:ymliu@chem.ecnu.edu.cn
  • Supported by:
    the National Natural Science Foundation of China(U1462106);Shanghai Leading Academic Discipline Project, China(B409)

摘要:

通过将杂原子B引入钛硅-1(TS-1)分子筛对其进行改性,并研究其催化氧化性能。结果发现,B-TS-1明显延长了环己酮氨肟化反应运行寿命。结合氨肟化体系催化剂失活主要原因以及反应体系H2O2反应路径,分析表明,H2O2是控制TS-1/H2O2氨肟化体系副反应发生的关键,并且有机副产物是导致催化剂堵孔失活的重要原因。本文提出B-TS-1能有效控制体系H2O2残留,从而进一步抑制副反应发生与积碳生成以延长催化剂寿命。结合Al-TS-1的催化特性,发现同时引入适量B、Al的B/Al-TS-1具有进一步提高环己酮肟化反应稳定性的作用。

关键词: B/Al-TS-1, 催化氧化, H2O2, 环己酮肟化, 失活

Abstract:

In this paper, boron-modified titanium silicalite-1 (B-TS-1) was synthesized, and its catalytic performance was studied. B-TS-1 improved the stability of cyclohexanone ammoximation. Combined with the root of deactivation of the catalyst and H2O2 reaction behavior in the liquid-phase ammoximation process, analysis showed that H2O2 is the key to control the side reactions of the cyclohexanone ammoximation system to form organic byproducts, and these byproducts result in the deactivation of catalyst because they block pores. It is concluded that B-TS-1 could effectively decrease the residual H2O2 to suppress the side reactions and prolong the catalyst lifetime in cyclohexanone ammoximation. Simultaneous introduction of appropriate amounts of B and Al to form B/Al-TS-1 resulted in a material that further improved the stability of cyclohexanone ammoximation.

Key words: B/Al-TS-1, Catalytic oxidation, H2O2, Cyclohexanone ammoximation, Deactivation

MSC2000: 

  • O643