TY - JOUR
T1 - Facile synthesis of the DD3R zeolite
T2 - Performance in the adsorptive separation of buta-1,3-diene and but-2-ene isomers
AU - Gücüyener, Canan
AU - Van Den Bergh, Johan
AU - Joaristi, Alberto Martinez
AU - Magusin, Pieter C.M.M.
AU - Hensen, Emiel J.M.
AU - Gascon, Jorge
AU - Kapteijn, Freek
PY - 2011/12/7
Y1 - 2011/12/7
N2 - Small pore size and hydrophobic nature of DD3R make this material a unique zeolite with high potential in industrial separation applications. However, the reproducible rapid synthesis of this zeolite is still a problem. In this work, a thorough assessment of different synthetic methods revealed that synthesis reproducibility relies on two main pillars: the use of properly cleaned autoclave liners and the synthesis composition. High quality DD3R crystals are obtained when KOH is used as a cleaning agent, eliminating memory effects, and when KF is used in the synthesis as a mineralizing agent. The effect of fluoride addition is investigated by use of several characterization techniques ( 13C, 19F and 29Si MAS-NMR and (2D) 29Si-1H correlation spectra), while monitoring the temporal crystallization of DDR. 29Si-1H NMR reveals that template molecules accommodated within the cages are sticking to these 8-ring windows through their amine group. High quality DD3R crystals are applied in the adsorptive separation of buta-1,3-diene and but-2-ene isomers, one of the most energy intensive separations in chemical industry. Mixture separation experiments revealed that the 8-ring apertures of the DD3R cages are only accessible to trans-but-2-ene and buta-1,3-diene, while excluding but-1-ene and cis-but-2-ene molecules, resulting in shape-selective separation in the presence of C4 mixtures.
AB - Small pore size and hydrophobic nature of DD3R make this material a unique zeolite with high potential in industrial separation applications. However, the reproducible rapid synthesis of this zeolite is still a problem. In this work, a thorough assessment of different synthetic methods revealed that synthesis reproducibility relies on two main pillars: the use of properly cleaned autoclave liners and the synthesis composition. High quality DD3R crystals are obtained when KOH is used as a cleaning agent, eliminating memory effects, and when KF is used in the synthesis as a mineralizing agent. The effect of fluoride addition is investigated by use of several characterization techniques ( 13C, 19F and 29Si MAS-NMR and (2D) 29Si-1H correlation spectra), while monitoring the temporal crystallization of DDR. 29Si-1H NMR reveals that template molecules accommodated within the cages are sticking to these 8-ring windows through their amine group. High quality DD3R crystals are applied in the adsorptive separation of buta-1,3-diene and but-2-ene isomers, one of the most energy intensive separations in chemical industry. Mixture separation experiments revealed that the 8-ring apertures of the DD3R cages are only accessible to trans-but-2-ene and buta-1,3-diene, while excluding but-1-ene and cis-but-2-ene molecules, resulting in shape-selective separation in the presence of C4 mixtures.
UR - http://www.scopus.com/inward/record.url?scp=80755159000&partnerID=8YFLogxK
U2 - 10.1039/c1jm13671b
DO - 10.1039/c1jm13671b
M3 - Article
AN - SCOPUS:80755159000
SN - 0959-9428
VL - 21
SP - 18386
EP - 18397
JO - Journal of Materials Chemistry
JF - Journal of Materials Chemistry
IS - 45
ER -