TY - JOUR
T1 - A time- and space-resolved catalyst deactivation study on the conversion of glycerol to aromatics using H-ZSM-5
AU - He, Songbo
AU - Goldhoorn, Hero Reinder
AU - Tegudeer, Zhuorigebatu
AU - Chandel, Anshu
AU - Heeres, Andre
AU - Stuart, Marc C.A.
AU - Heeres, Hero Jan
N1 - Funding Information:
Financial support from Netherlands Organization for Scientific Research (NWO-LIFT programme, Grant No.731.016.401) is greatly acknowledged. We also acknowledge BioBTX B.V. for stimulating discussions and valuable input.
Publisher Copyright:
© 2022 The Authors
PY - 2022/4/15
Y1 - 2022/4/15
N2 - A time- and space-resolved deactivation study on the conversion of glycerol to aromatics over H-ZSM-5 was performed. For this purpose, glycerol was vaporized/pyrolyzed in a pyrolysis section followed by a catalytic aromatization step. Benchmark performance showed an induction period of ca. 20 min, followed by a rather constant BTX yield of ca. 25.4 ± 2.2C.% for 3–4 h time on stream (TOS). Subsequently, a rapid drop in BTX yield was observed due to catalyst deactivation. Severe coking leads to coverage of catalyst surface area and blockage of micropores, particularly at the entrance of the catalyst bed at short TOS, indicating the presence of an axial coke gradient in the fixed bed reactor. At longer TOS, coke was formed throughout the bed and negligible BTX yield was shown to be associated with the presence of coke at all bed positions. Besides coking, the acidity of the catalyst was also reduced, and dealumination occurred, both with a similar time–space evolution. The results were explained by a conversion-zone migration model, which includes a deactivation zone (with severely coked catalyst), a conversion zone (BTX formation), and an induction zone (a.o. (de-)alkylation reactions), and describes the time- and space-resolved evolution of coking and relevant changes in other catalyst characteristics.
AB - A time- and space-resolved deactivation study on the conversion of glycerol to aromatics over H-ZSM-5 was performed. For this purpose, glycerol was vaporized/pyrolyzed in a pyrolysis section followed by a catalytic aromatization step. Benchmark performance showed an induction period of ca. 20 min, followed by a rather constant BTX yield of ca. 25.4 ± 2.2C.% for 3–4 h time on stream (TOS). Subsequently, a rapid drop in BTX yield was observed due to catalyst deactivation. Severe coking leads to coverage of catalyst surface area and blockage of micropores, particularly at the entrance of the catalyst bed at short TOS, indicating the presence of an axial coke gradient in the fixed bed reactor. At longer TOS, coke was formed throughout the bed and negligible BTX yield was shown to be associated with the presence of coke at all bed positions. Besides coking, the acidity of the catalyst was also reduced, and dealumination occurred, both with a similar time–space evolution. The results were explained by a conversion-zone migration model, which includes a deactivation zone (with severely coked catalyst), a conversion zone (BTX formation), and an induction zone (a.o. (de-)alkylation reactions), and describes the time- and space-resolved evolution of coking and relevant changes in other catalyst characteristics.
KW - BTX
KW - Catalyst deactivation
KW - Coke
KW - Conversion-zone migration model
KW - Dealumination
KW - Glycerol
UR - http://www.scopus.com/inward/record.url?scp=85123094064&partnerID=8YFLogxK
U2 - 10.1016/j.cej.2022.134620
DO - 10.1016/j.cej.2022.134620
M3 - Article
AN - SCOPUS:85123094064
SN - 1385-8947
VL - 434
JO - Chemical Engineering Journal
JF - Chemical Engineering Journal
M1 - 134620
ER -