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Hydrodechlorination of 1,2-dichloroethane on nickel loaded Beta zeolite modified by copper: Influence of nickel and copper state on product selectivity

Paper ID Volume ID Publish Year Pages File Format Full-Text
54518 47012 2014 7 PDF Available
Title
Hydrodechlorination of 1,2-dichloroethane on nickel loaded Beta zeolite modified by copper: Influence of nickel and copper state on product selectivity
Abstract

•Two-step postsynthesis method is a very effective way to obtain catalysts with high metal dispersion.•Red-C-Ni2.0SiBEA and red-C-Cu2.0Ni2.0SiBEA catalyst are active in HDC of 1,2-dichloroethane.•HRTEM of red-C-Cu2.0Ni2.0SiBEA allowed distinguishing separately Ni and Cu nanoparticles.•Red-C-Cu2.0Ni2.0SiBEA catalyst shows excellent selectivity toward ethylene (∼96%).

Influence of copper addition to nickel containing zeolite on activity and product selectivity in the hydrodechlorination of 1,2-dichloroethane was investigated. Ni2.0SiBEA and Cu2.0Ni2.0SiBEA zeolites were prepared by a two-steps postsynthesis method which consist of (1) creation of vacant T-atom sites by dealumination of calcined BEA zeolite with nitric acid and then (2) impregnation of as resulting SiBEA with aqueous nickel nitrate solution or co-impregnation with aqueous nickel and copper nitrate solution, respectively. Calcination at 773 K for 3 h in air and then reduction at 873 K over 3 h in flowing 10% H2/Ar of Ni2.0SiBEA and Cu2.0Ni2.0SiBEA, with an isolated pseudo-tetrahedral Ni(II) and Cu(II) species incorporated into BEA framework, leads to formation of red-C-Ni2.0SiBEA and red-C-Cu2.0Ni2.0SiBEA catalysts with very well dispersed metal nanoparticles. The state of nickel and copper in catalysts after calcination, reduction and reaction was characterized by XRD, low-temperature N2 sorption, TPR and XPS. The red-C-Ni2.0SiBEA and red-C-Cu2.0Ni2.0SiBEA catalysts were active in hydrodechlorination of 1,2-dichloroethane with very high selectivity into ethylene (90 and 96% respectively), desired product of this reaction. Thus, the simultaneous introduction of copper and nickel ions in SiBEA in the second step of postsynthesis procedure allows obtaining bimetallic red-C-Cu2.0Ni2.0SiBEA catalyst with well dispersed, separated Cu and Ni particles with higher selectivity toward ethylene than red-C-Ni2.0SiBEA catalyst. TEM experiments have shown that after catalytic run a very small agglomeration of metal particles took place. According to TPH and XPS measurements chlorine containing species are present in spent zeolite catalysts.

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Keywords
Ni; Cu; SiBEA; Hydrodechlorination; 1,2-Dichloroethane
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Hydrodechlorination of 1,2-dichloroethane on nickel loaded Beta zeolite modified by copper: Influence of nickel and copper state on product selectivity
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Publisher
Database: Elsevier - ScienceDirect
Journal: Catalysis Today - Volume 226, 1 May 2014, Pages 134–140
Authors
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Subjects
Physical Sciences and Engineering Chemical Engineering Catalysis
Get Full-Text Now
Don't Miss Today's Special Offer
Price was $35.95
You save - $31
Price after discount Only $4.95
100% Money Back Guarantee
Full-text PDF Download
Online Support
Any Questions? feel free to contact us