In Situ Aluminum Migration into Zeolite Framework during Methanol-To-Propylene Reaction: An Innovation to Design Superior Catalysts

Junjie Li, Min Liu, Xinwen Guo, Chengyi Dai, Shutao Xu, Yingxu Wei, Zhongmin Liu, Chunshan Song

Research output: Contribution to journalArticle

4 Citations (Scopus)

Abstract

This work involves methanol-to-propylene (MTP) conversion over aluminosilicate MFI (ZSM-5), borosilicate MFI (B-ZSM-5), and all-silica MFI (Silicate-1). Both B-ZSM-5 and Silicate-1 were inactive in MTP reaction. However, extruded Silicate-1 sample prepared by extrusion with Al2O3 binder, followed by acid washing treatment, displayed a rapid increase in methanol conversion in the initial 30 h time on stream (TOS), and then retained 99% methanol conversion, higher propylene selectivity (52.2%), and higher propylene/ethylene ratio (11.3) for 400 h TOS. Silicate-1 modified with AlCl3 or Al(NO3)3 showed similar catalytic performance as the extruded samples. Several AlCl3-modified Silicate-1 samples after various TOS values were regenerated and characterized by NH3-termperature-programmed desorption (TPD), Fourier transform infrared (FT-IR) spectroscopy, and 27Al magic angle spinning nuclear magnetic responance (MAS NMR). The results point to continuous aluminum insertion into Silicate-1 framework during reaction in situ, which rationalizes the superior catalytic performance. By analyzing catalytic performances of AlCl3-modified samples with different amounts of defect sites, we concluded that Al migration is related to the defect sites. Finally, a catalyst with a much longer lifetime of 960 h and 53.2% propylene selectivity was developed by incorporating Al migration into hierarchical samples.

Original languageEnglish (US)
Pages (from-to)8190-8199
Number of pages10
JournalIndustrial and Engineering Chemistry Research
Volume57
Issue number24
DOIs
StatePublished - Jun 20 2018

Fingerprint

Zeolites
Silicates
Aluminum
Propylene
Methanol
Innovation
Catalysts
Defects
Magic angle spinning
Aluminosilicates
Washing
Silicon Dioxide
Binders
Fourier transform infrared spectroscopy
Extrusion
propylene
Desorption
Ethylene
Silica
Acids

All Science Journal Classification (ASJC) codes

  • Chemistry(all)
  • Chemical Engineering(all)
  • Industrial and Manufacturing Engineering

Cite this

Li, Junjie ; Liu, Min ; Guo, Xinwen ; Dai, Chengyi ; Xu, Shutao ; Wei, Yingxu ; Liu, Zhongmin ; Song, Chunshan. / In Situ Aluminum Migration into Zeolite Framework during Methanol-To-Propylene Reaction : An Innovation to Design Superior Catalysts. In: Industrial and Engineering Chemistry Research. 2018 ; Vol. 57, No. 24. pp. 8190-8199.
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abstract = "This work involves methanol-to-propylene (MTP) conversion over aluminosilicate MFI (ZSM-5), borosilicate MFI (B-ZSM-5), and all-silica MFI (Silicate-1). Both B-ZSM-5 and Silicate-1 were inactive in MTP reaction. However, extruded Silicate-1 sample prepared by extrusion with Al2O3 binder, followed by acid washing treatment, displayed a rapid increase in methanol conversion in the initial 30 h time on stream (TOS), and then retained 99{\%} methanol conversion, higher propylene selectivity (52.2{\%}), and higher propylene/ethylene ratio (11.3) for 400 h TOS. Silicate-1 modified with AlCl3 or Al(NO3)3 showed similar catalytic performance as the extruded samples. Several AlCl3-modified Silicate-1 samples after various TOS values were regenerated and characterized by NH3-termperature-programmed desorption (TPD), Fourier transform infrared (FT-IR) spectroscopy, and 27Al magic angle spinning nuclear magnetic responance (MAS NMR). The results point to continuous aluminum insertion into Silicate-1 framework during reaction in situ, which rationalizes the superior catalytic performance. By analyzing catalytic performances of AlCl3-modified samples with different amounts of defect sites, we concluded that Al migration is related to the defect sites. Finally, a catalyst with a much longer lifetime of 960 h and 53.2{\%} propylene selectivity was developed by incorporating Al migration into hierarchical samples.",
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In Situ Aluminum Migration into Zeolite Framework during Methanol-To-Propylene Reaction : An Innovation to Design Superior Catalysts. / Li, Junjie; Liu, Min; Guo, Xinwen; Dai, Chengyi; Xu, Shutao; Wei, Yingxu; Liu, Zhongmin; Song, Chunshan.

In: Industrial and Engineering Chemistry Research, Vol. 57, No. 24, 20.06.2018, p. 8190-8199.

Research output: Contribution to journalArticle

TY - JOUR

T1 - In Situ Aluminum Migration into Zeolite Framework during Methanol-To-Propylene Reaction

T2 - An Innovation to Design Superior Catalysts

AU - Li, Junjie

AU - Liu, Min

AU - Guo, Xinwen

AU - Dai, Chengyi

AU - Xu, Shutao

AU - Wei, Yingxu

AU - Liu, Zhongmin

AU - Song, Chunshan

PY - 2018/6/20

Y1 - 2018/6/20

N2 - This work involves methanol-to-propylene (MTP) conversion over aluminosilicate MFI (ZSM-5), borosilicate MFI (B-ZSM-5), and all-silica MFI (Silicate-1). Both B-ZSM-5 and Silicate-1 were inactive in MTP reaction. However, extruded Silicate-1 sample prepared by extrusion with Al2O3 binder, followed by acid washing treatment, displayed a rapid increase in methanol conversion in the initial 30 h time on stream (TOS), and then retained 99% methanol conversion, higher propylene selectivity (52.2%), and higher propylene/ethylene ratio (11.3) for 400 h TOS. Silicate-1 modified with AlCl3 or Al(NO3)3 showed similar catalytic performance as the extruded samples. Several AlCl3-modified Silicate-1 samples after various TOS values were regenerated and characterized by NH3-termperature-programmed desorption (TPD), Fourier transform infrared (FT-IR) spectroscopy, and 27Al magic angle spinning nuclear magnetic responance (MAS NMR). The results point to continuous aluminum insertion into Silicate-1 framework during reaction in situ, which rationalizes the superior catalytic performance. By analyzing catalytic performances of AlCl3-modified samples with different amounts of defect sites, we concluded that Al migration is related to the defect sites. Finally, a catalyst with a much longer lifetime of 960 h and 53.2% propylene selectivity was developed by incorporating Al migration into hierarchical samples.

AB - This work involves methanol-to-propylene (MTP) conversion over aluminosilicate MFI (ZSM-5), borosilicate MFI (B-ZSM-5), and all-silica MFI (Silicate-1). Both B-ZSM-5 and Silicate-1 were inactive in MTP reaction. However, extruded Silicate-1 sample prepared by extrusion with Al2O3 binder, followed by acid washing treatment, displayed a rapid increase in methanol conversion in the initial 30 h time on stream (TOS), and then retained 99% methanol conversion, higher propylene selectivity (52.2%), and higher propylene/ethylene ratio (11.3) for 400 h TOS. Silicate-1 modified with AlCl3 or Al(NO3)3 showed similar catalytic performance as the extruded samples. Several AlCl3-modified Silicate-1 samples after various TOS values were regenerated and characterized by NH3-termperature-programmed desorption (TPD), Fourier transform infrared (FT-IR) spectroscopy, and 27Al magic angle spinning nuclear magnetic responance (MAS NMR). The results point to continuous aluminum insertion into Silicate-1 framework during reaction in situ, which rationalizes the superior catalytic performance. By analyzing catalytic performances of AlCl3-modified samples with different amounts of defect sites, we concluded that Al migration is related to the defect sites. Finally, a catalyst with a much longer lifetime of 960 h and 53.2% propylene selectivity was developed by incorporating Al migration into hierarchical samples.

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