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Acta Phys. -Chim. Sin.  2016, Vol. 32 Issue (10): 2574-2580    DOI: 10.3866/PKU.WHXB201606294
ARTICLE     
Synthesis and Catalytic Oxidation Performance of B-TS-1
Lei WANG,Han-Mei YIN,Jian-Hao WANG,Li-Zhi WU,Yue-Ming LIU*()
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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 wordsB/Al-TS-1      Catalytic oxidation      H2O2      Cyclohexanone ammoximation      Deactivation     
Received: 03 May 2016      Published: 29 June 2016
MSC2000:  O643  
Fund:  the National Natural Science Foundation of China(U1462106);Shanghai Leading Academic Discipline Project, China(B409)
Corresponding Authors: Yue-Ming LIU     E-mail: ymliu@chem.ecnu.edu.cn
Cite this article:

Lei WANG,Han-Mei YIN,Jian-Hao WANG,Li-Zhi WU,Yue-Ming LIU. Synthesis and Catalytic Oxidation Performance of B-TS-1. Acta Phys. -Chim. Sin., 2016, 32(10): 2574-2580.

URL:

http://www.whxb.pku.edu.cn/10.3866/PKU.WHXB201606294     OR     http://www.whxb.pku.edu.cn/Y2016/V32/I10/2574

Fig 1  XRD patterns of B/Al-TS-160 (a) TS-1; (b) B90-TS-1; (c) Al90-TS-1. Bx/Aly-TS-1z: x represents the Si/B molar ratio; y represents the Si/Al molar ratio; z represents the Si/Ti molar ratio.
Fig 2  UV-Vis spectra of B/Al-TS-160 with different compositions (a) TS-1; (b) B90-TS-1; (c) B30-TS-1; (d) Al150-TS-1; (e) Al90-TS-1
Fig 3  Composition of different B/Al-TS-1 measured by ICP (A) B30-TS-1: (a) Si/B; (b) Si/Ti; (c) Si/(Ti + B). (B) Al-TS-160: (a)Si/Al; (b) Si/Ti; (c) Si/(Ti + Al). ICP: inductively coupled plasma
Fig 4  SEM images of B/Al-TS-160 (a) TS-1; (b) B90-TS-1; (c) Al90-TS-1
Fig 5  Effect of different component ratio of B/Al-TS-1 on the epoxidation of hexene (A) B-TS-160: (a) B60,(b) B90,(c) B120,(d) B150,(e) TS-1; (B) Al-TS-160: (a) Al90,(b) Al120,(c) Al300,(d) Al500,(e) TS-1
Fig 6  Lifetime of B/Al-TS-1 with different Si/B and Si/Al molar ratios in ammoximation of cyclohexanone (a) TS-1; (b) B90-TS-1; (c) Al90-TS-1; (d) B90-Al90-TS-1
Fig 7  Comparison of running status of ammoximation of cyclohexanone under the condition of different nH2O2 /nketone ratios nH2O2 /nketone: (a) 1.05; (b) 1.10; (c) 1.20; (d) 1.30
Fig 8  Lifetime of TS-160 (a,b) and B90-TS-160 (c,d) in the ammoximation of cyclohexanone with different nH2O2 /nketone ratios nH2O2 /nketone: (a,c) 1.10; (b,d) 1.20
No.SamplenH2O2/nketonew(residual H2O2)/%
t1t2t3
1TS-1601.050.160.200.18
2TS-1601.100.180.230.49
3TS-1601.200.180.410.37
4TS-1601.300.460.500.55
5B90-TS-1601.200.190.190.39
Table 1  Analysis of concentration of residual H2O2 of TS-160 & B90-TS-160 in the ammoximation of cyclohexanone
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