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Frontiers of Chemical Science and Engineering

ISSN 2095-0179

ISSN 2095-0187(Online)

CN 11-5981/TQ

邮发代号 80-969

2019 Impact Factor: 3.552

Frontiers of Chemical Science and Engineering  2024, Vol. 18 Issue (11): 129   https://doi.org/10.1007/s11705-024-2481-6
  本期目录
Kinetics of hydroxylation of phenol with SiC foam supported TS-1 structured catalyst
Yanzhao Sun1,2, Zhitao Lv1,2, Siyu Zhang1,2, Guodong Wen1(), Yilai Jiao1()
1. Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, China
2. School of Materials Science and Engineering, University of Science and Technology of China, Shenyang 110016, China
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Abstract

In light of the challenges associated with catalyst separation and recovery, as well as the low production efficiency resulting from intermittent operation for titanium silicalite-1 (TS-1) catalyzed phenol hydroxylation to dihydroxybenzene in the slurry bed, researchers keep on exploring the use of a continuous fixed bed to replace the slurry bed process in recent years. This study focuses on preparing a TS-1 coated structured catalyst on SiC foam, which exhibits significant process intensification in performance. We investigated the kinetics of this structured catalyst and compared it with those of extruded TS-1 catalyst; the dynamic equations of the two catalysts were obtained. It was observed that both catalysts followed E-R adsorption mechanism model, with an effective internal diffusion factor ratio between structured and extruded TS-1 of approximately 7.71. It was confirmed that the foamed SiC-based structured TS-1 catalyst exhibited significant improvements in phenol hydroxylation in fixed-bed reactor due to its well-developed pore structure, good thermal conductivity, excellent internal mass transfer performance, and short reactant diffusion distance, leading to higher utilization efficiency of active components. This finding also provides a foundation for designing and developing phenol hydroxylation processes in fixed-bed using structured catalysts through computational fluid dynamics calculations.

Key wordstitanium silicalite-1    phenol hydroxylation    SiC foam    structured catalyst    coating
收稿日期: 2024-03-23      出版日期: 2024-08-13
Corresponding Author(s): Guodong Wen,Yilai Jiao   
 引用本文:   
. [J]. Frontiers of Chemical Science and Engineering, 2024, 18(11): 129.
Yanzhao Sun, Zhitao Lv, Siyu Zhang, Guodong Wen, Yilai Jiao. Kinetics of hydroxylation of phenol with SiC foam supported TS-1 structured catalyst. Front. Chem. Sci. Eng., 2024, 18(11): 129.
 链接本文:  
https://academic.hep.com.cn/fcse/CN/10.1007/s11705-024-2481-6
https://academic.hep.com.cn/fcse/CN/Y2024/V18/I11/129
Fig.1  
Serial number 1 2 3 4 5 6 7 8 9 10
Cp/(mol·L–1) 0.5300 0.5300 0.5300 0.5300 0.6360 0.6890 0.7420 0.5300 0.5300 0.5300
CH/(mol·L–1) 0.0530 0.0530 0.0530 0.0530 0.0530 0.0530 0.0530 0.0297 0.0396 0.0594
T/K 338 343 348 353 353 353 353 353 353 353
Tab.1  
Sample SBETa)/(m2·g–1) Smicrob)/(m2·g–1) Sextb)/(m2·g–1) Vmicrob)/(cm3·g–1) Vmesoc)/(cm3·g–1)
TS-1-Powder 477.70 443.95 33.75 0.1747 0.1301
TS-1-Structured 56.67 42.65 14.02 0.0198 0.0375
TS-1-Extruded 382.59 304.35 78.24 0.1247 0.2472
TS-1 coatingd) 396.69 298.55 98.14 0.1386 0.2625
Tab.2  
Fig.2  
Fig.3  
Fig.4  
Fig.5  
Fig.6  
Fig.7  
Mechanism TS-1-Structured TS-1-Extruded
Langmuir-Hinshelwood k 3.02×102exp(?34.26RT) 1.93×104exp(?8.86×103RT)
bH 3.64×10?2exp(47.36RT) 1.66×10?4exp(2.55×104RT)
bP 3.07×10?8exp(7.29×104RT) 1.78exp(39.86RT)
Eley-Rideal k 2.18×103exp(?1.34×104RT) 1.76×103exp(?1.56×104RT)
bH 1.09×10?2exp(3.65×103RT) 1.19×10?2exp(1.27×103RT)
bP 2.35×10?3exp(1.06×103RT) 7.80×10?3exp(2.66RT)
Tab.3  
RSS R2
L-H E-R L-H E-R
TS-1-Structured 0.02063 0.00133 0.8466 0.9899
TS-1-Extruded 0.09306 0.00821 0.2986 0.9381
Tab.4  
Fig.8  
1 B Bukowska , J Michalowicz , A Marczak . The effect of catechol on human peripheral blood mononuclear cells (in vitro study). Environmental Toxicology and Pharmacology, 2015, 39(1): 187–193
https://doi.org/10.1016/j.etap.2014.11.017
2 J Iniesta , P A Michaud , M Panizza , G Cerisola , A Aldaz , C Comninellis . Electrochemical oxidation of phenol at boron-doped diamond electrode. Electrochimica Acta, 2001, 46(23): 3573–3578
https://doi.org/10.1016/S0013-4686(01)00630-2
3 K C Gupta , A K Sutar . Polymer supported catalysts for oxidation of phenol and cyclohexene using hydrogen peroxide as oxidant. Journal of Molecular Catalysis A Chemical, 2008, 280(1-2): 173–185
https://doi.org/10.1016/j.molcata.2007.11.007
4 H N Shi , Y Q Wang , G Q Wu , W P Feng , Y Lin , T Zhang , X Jin , S H Wang , X X Wu , P X Yao . Deactivation and regeneration of TS-1/SiO2 catalyst for epoxidation of propylene with hydrogen peroxide in a fixed-bed reactor. Frontiers of Chemical Science and Engineering, 2013, 7(2): 202–209
https://doi.org/10.1007/s11705-013-1328-3
5 J Xu , Y Q Wang , W P Feng , Y Lin , S H Wang . Effect of triethylamine treatment of titanium silicalite-1 on propylene epoxidation. Frontiers of Chemical Science and Engineering, 2014, 8(4): 478–487
https://doi.org/10.1007/s11705-014-1453-7
6 P X Yao , Y Q Wang , T Zhang , S H Wang , X X Wu . Effect of sodium ions in synthesis of titanium silicalite-1 on its catalytic performance for cyclohexanone ammoximation. Frontiers of Chemical Science and Engineering, 2014, 8(2): 149–155
https://doi.org/10.1007/s11705-014-1409-y
7 B Y Liu , Q W Mu , J J Huang , W Tan , J Xiao . Fabrication of titanosilicate pillared MFI zeolites with tailored catalytic activity. Frontiers of Chemical Science and Engineering, 2020, 14(5): 772–782
https://doi.org/10.1007/s11705-019-1859-3
8 G Vega , A Quintanilla , M Belmonte , J A Casas . Kinetic study of phenol hydroxylation by H2O2 in 3D Fe/SiC honeycomb monolithic reactors: enabling the sustainable production of dihydroxybenzenes. Chemical Engineering Journal, 2022, 428: 9–17
https://doi.org/10.1016/j.cej.2021.131128
9 S B Dehghanpour , M Razavi , F Parvizian . Synthesis of ultra-fine TS-1 catalyst with high titanium content and its performance in phenol hydroxylation. New Journal of Chemistry, 2023, 47(42): 19439–19446
https://doi.org/10.1039/D3NJ03744D
10 H Li , Y Zhai , X B Zhang , G J Lv , Y Shen , X Q Wang , T Jiang , Y Z Wu . Iron-containing TS-1 zeolites with controllable mesopores by desilication and their application in phenol hydroxylation. Industrial & Engineering Chemistry Research, 2020, 59(22): 10289–10297
https://doi.org/10.1021/acs.iecr.0c00048
11 Z Y Yang , Y N Guan , L Xu , Y T Zhou , X L Fan , Y L Jiao . Tetrapropylammonium hydroxide treatment of aged dry gel to make hierarchical TS-1 zeolites for catalysis. Crystal Growth & Design, 2023, 23(3): 1775–1785
https://doi.org/10.1021/acs.cgd.2c01291
12 L Zong , Y Liu , F Xin . In situ synthesis of titanium silicalite-1 on monolithic cordierite support. Journal of Inorganic Materials, 2007, 22: 1227–1232
13 X H Liu , C Y Yang , Y Q Wang , Y L Guo , Y Guo , G Z Lu . Effect of the diatomite pretreatment on the catalytic performance of TS-1/diatomite for toluene hydroxylation by H2O2 in fixed-bed reactor. Chemical Engineering Journal, 2014, 243: 192–196
https://doi.org/10.1016/j.cej.2013.12.055
14 G Q Liu , J G Kuang , J Wu , H A Luo . Synthesis and characterization of extruded titanium silicate-1 and its catalysis performance in cyclohexanone ammoximation. Chemical Reaction Engineering and Technology, 2010, 26: 42–46
15 G Vega , A Quintanilla , N Menendez , M Belmonte , J A Casas . 3D honeycomb monoliths with interconnected channels for the sustainable production of dihydroxybenzenes: towards the intensification of selective oxidation processes. Chemical Engineering and Processing-Process Intensification, 2021, 165: 13–25
https://doi.org/10.1016/j.cep.2021.108437
16 Y L Jiao , X D Yang , C H Jiang , C Tian , Z M Yang , J S Zhang . Hierarchical ZSM-5/SiC nano-whisker/SiC foam composites: preparation and application in MTP reactions. Journal of Catalysis, 2015, 332: 70–76
https://doi.org/10.1016/j.jcat.2015.09.002
17 Q Y Ding , H Y Shen , Z L Kou , H Li , X L Fan , X X Ou , Y L Jiao , X Gao . Heteropoly acid supported on hierarchical Y zeolite decorated SiC foam as the structured catalytic packing for reactive distillation synthesis of ethyl lactate. Chemical Engineering Journal, 2023, 476: 146493
https://doi.org/10.1016/j.cej.2023.146493
18 Y N Guan , Y T Zhou , C H Jiang , X X Xu , Z M Yang , J S Zhang , X L Fan , Y L Jiao . Catalytic combustion of volatile organic compounds (VOCs) over structured Co3O4 nano-flowers on silicalite-1/SiC foam catalysts. Microporous and Mesoporous Materials, 2021, 323: 12–23
https://doi.org/10.1016/j.micromeso.2021.111173
19 X D Yang , C H Jiang , Z M Yang , J S Zhang . Hydrochlorination of acetylene using SiC foam supported structured C/Au catalysts. Journal of Materials Science and Technology, 2014, 30(5): 434–440
https://doi.org/10.1016/j.jmst.2014.01.013
20 H Liu , G Z Lu , Y L Guo , Y Guo , J S Wang . Chemical kinetics of hydroxylation of phenol catalyzed by TS-1/diatomite in fixed-bed reactor. Chemical Engineering Journal, 2006, 116(3): 179–186
https://doi.org/10.1016/j.cej.2005.12.001
21 A V Sulimov , S M Danov , A V Ovcharova , A A Ovcharov , V R Flid . Kinetics of allyl chloride epoxidation with hydrogen peroxide catalyzed by extruded titanium silicalite. Kinetics and Catalysis, 2014, 55(6): 712–721
https://doi.org/10.1134/S0023158414060135
22 R Klaewkla , S Kulprathipanja , P Rangsunvigit , T Rirksomboon , W Rathbun , L Nemeth . Kinetic modelling of phenol hydroxylation using titanium and tin silicalite-1s: effect of tin incorporation. Chemical Engineering Journal, 2007, 129(1-3): 21–30
https://doi.org/10.1016/j.cej.2006.10.034
23 D E Mears . Tests for transport limitations in experimental catalytic reactors. Industrial & Engineering Chemistry Process Design and Development, 1971, 10(4): 541–547
https://doi.org/10.1021/i260040a020
24 M Wen , J Ding , C Z Wang , Y K Li , G F Zhao , Y Liu , Y Lu . High-performance SS-fiber@HZSM-5 core shell catalyst for methanol-to-propylene: a kinetic and modeling study. Microporous and Mesoporous Materials, 2016, 221: 187–196
https://doi.org/10.1016/j.micromeso.2015.09.039
25 M Liu , X W Guo , X S Wang . Highly effective phenol hydroxylation over Ti-ZSM-5 catalyst prepared using B-ZSM-5 as precursor. Chinese Journal of Catalysis, 2004, 25: 169–170
26 H J Zhang , M K Yao , W Xie , Y M Liu , P Wu . Synthesis of TS-1 using inorganic SiO2-TiO2 precursor and its catalytic performance for hydroxylation of phenol. Chinese Journal of Catalysis, 2007, 28: 895–899
27 A Tuel , S Moussa-Khouzami , Y B Taarit , C Naccache . Hydroxylation of phenol over TS-1: surface and solvent effects. Journal of Molecular Catalysis, 1991, 68(1): 45–52
https://doi.org/10.1016/0304-5102(91)80060-G
28 G Q Wu , Z G Lin , L Li , L Zhang , Y P Hong , W J Wang , C Chen , Y Jiang , X Z Yan . Experiments and kinetics of the epoxidation of allyl chloride with H2O2 over organic base treated TS-1 catalysts. Chemical Engineering Journal, 2017, 320: 1–10
https://doi.org/10.1016/j.cej.2017.03.030
29 H Liu , G Z Lu , Y L Guo , Y Guo , J S Wang . Catalytic performance of titanium silicalite-1 for hydroxylation of phenol in fixed-bed reactor. Chinese Journal of Catalysis, 2004, 25: 49–54
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