Kinetics of hydroxylation of phenol with SiC foam supported TS-1 structured catalyst

doi:10.1007/s11705-024-2481-6

Front. Chem. Sci. Eng.

2024, Vol. 18

Issue (11) : 129 https://doi.org/10.1007/s11705-024-2481-6

Kinetics of hydroxylation of phenol with SiC foam supported TS-1 structured catalyst

Yanzhao Sun^1,², Zhitao Lv^1,², Siyu Zhang^1,², 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.

Keywords titanium silicalite-1 phenol hydroxylation SiC foam structured catalyst coating

Corresponding Author(s): Guodong Wen,Yilai Jiao

About author:

^#These authors contributed equally to this work.

Just Accepted Date: 31 May 2024 Issue Date: 13 August 2024

Cite this article:

Yanzhao Sun,Zhitao Lv,Siyu Zhang, et al. Kinetics of hydroxylation of phenol with SiC foam supported TS-1 structured catalyst[J]. Front. Chem. Sci. Eng., 2024, 18(11): 129.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-024-2481-6
https://academic.hep.com.cn/fcse/EN/Y2024/V18/I11/129

Fig.1 (a) Macro structure of TS-1-Structured; (b, c) SEM morphology of the interface of the SiC foam and TS-1 coatings; (d) XRD patterns of TS-1-Powder, TS-1-Structured and SiC foam; (e) N₂ adsorption and desorption curves of TS-1-Powder, TS-1-Structured, TS-1-Extruded and SiC foam; (f) cumulative pore volume and pore size distribution of TS-1-Structured and TS-1-Extruded by mercury intrusion.

Tab.1 Summary of reaction conditions involved in the study of phenol hydroxylation kinetics^a)

Tab.2 Structural parameters of TS-1-Powder, TS-1-Structured, TS-1-Extruded and TS-1 coating

Fig.2 (a) The phenol conversion and (b) the selectivity of products against the space time over TS-1-Structured and TS-1-Extruded.

Fig.3 Relationship between temperature and (a) initial reaction rate of phenol and (b) initial conversion rate of phenol.

Fig.4 The relationship between the concentration of H₂O₂ and (a) the initial reaction rate of phenol hydroxylation and (b) the initial conversion rate of phenol.

Fig.5 The relationship between phenol concentration and (a) initial phenol hydroxylation rate and (b) initial phenol conversion rate.

Fig.6 Numerical test of kinetic equations of (a) TS-1-Structured and (b) TS-1-Extruded power functions.

Fig.7 Reaction routes involved in hydroxylation of phenol on TS-1.

Mechanism		TS-1-Structured	TS-1-Extruded
Langmuir-Hinshelwood	k	$3.02 × 102 e x p (? 34.26 R T)$	$1.93 × 104 e x p (? 8.86 × 103 R T)$
	b_H	$3.64 × 10 ? 2 e x p (47.36 R T)$	$1.66 × 1 0 ? 4 e x p (2.55 × 104 R T)$
	b_P	$3.07 × 1 0 ? 8 e x p (7.29 × 104 R T)$	$1.78 e x p (39.86 R T)$
Eley-Rideal	k	$2.18 × 103 e x p (? 1.34 × 104 R T)$	$1.76 × 103 e x p (? 1.56 × 104 R T)$
	b_H	$1.09 × 10 ? 2 e x p (3.65 × 103 R T)$	$1.19 × 10 ? 2 e x p (1.27 × 103 R T)$
	b_P	$2.35 × 10 ? 3 e x p (1.06 × 103 R T)$	$7.80 × 10 ? 3 e x p (2.66 R T)$

Tab.3 Reaction rate equation parameters of the two mechanisms

Tab.4 Statistical test of two reaction mechanism models

Fig.8 Reactor bed temperature comparison between TS-1-Structured and TS-1-Extruded at a space time of 94.63 g_zeolite·h·mol_phenol^–1.

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