失活TS-1高效催化C=4裂解制C=3反应的研究

Xin Huang; Yuxia Lin; Binghui Yan; Yueming Liu

doi:10.11949/0438-1157.20210506

失活TS-1高效催化C⁼₄裂解制C⁼₃反应的研究

Translated title of the contribution: Deactivated TS-1 as an efficient catalyst for catalytic cracking of butene to propene

Xin Huang
, Yuxia Lin
, Binghui Yan
, Yueming Liu^*

^*Corresponding author for this work

School of Chemistry and Molecular Engineering

East China Normal University

Research output: Contribution to journal › Article › peer-review

6 Scopus citations

Abstract

Catalytic cracking of light olefins (C⁼₄/C⁼₅) can produce high value-added product C⁼₃, meanwhile achieve efficient utilization of C₄/C₅ resources, which has very important research significance and industrial application value. The main technical problem of catalytic cracking of C⁼₄ is how to obtain high selectivity of olefin products, especially the target product C⁼₃ and to reduce non-olefin by-products, and its core lies in the development of high-efficiency catalysts. At present, the main industrial catalyst is modified ZSM-5. Titanium silicate molecular sieve TS-1 is a high-efficiency catalyst in the liquid phase ammoximation process of industrial cyclohexanone, which shows a typical Brønsted acid property after deactivation. Based on this, the deactivated TS-1 as an efficient catalyst for catalytic cracking of C⁼₄ to produce C⁼₃ was developed, and the result indicated that the deactivated TS-1 after acid treatment and potassium ion (K⁺) exchange could show the feature of high activity, high selectivity and high stability. Combined with nitric acid treating modification, K⁺ exchange experiment and the characterization techniques such as UV-Vis (UV-visible spectroscopy), FT-IR (Fourier transform infrared spectrometer) and NH₃-TPD (temperature-programmed desorption of ammonia), it was found that the catalytic cracking active center of deactivated TS-1 is Brønsted acidic silyl hydroxyl group (Si-OH(Ti)) adjacent to the titanium hydroxyl group. The structure of this Brønsted acid site is completely different from the skeleton bridge Brønsted acid site (Si-(OH)-Al) of ZSM-5, meanwhile shows relatively weak acid strength. The unique acid property of Si-OH(Ti) could promote the main reaction path of catalytic cracking of C⁼₄ to produce C⁼₃ and inhibit the side reaction path of hydrogen transfer reaction. The discovery and application of the special Brønsted acid center of the deactivated TS-1 waste catalyst can provide a new idea for resource utilization of solid waste resources of spent catalyst.

Translated title of the contribution	Deactivated TS-1 as an efficient catalyst for catalytic cracking of butene to propene
Original language	Chinese (Traditional)
Pages (from-to)	5183-5195
Number of pages	13
Journal	Huagong Xuebao/CIESC Journal
Volume	72
Issue number	10
DOIs	https://doi.org/10.11949/0438-1157.20210506
State	Published - Oct 2021

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

Access to Document

10.11949/0438-1157.20210506

Cite this

@article{201333a98d4642aeaad91dc85ffe1120,

title = "失活TS-1高效催化C=4裂解制C=3反应的研究",

abstract = "Catalytic cracking of light olefins (C=4/C=5) can produce high value-added product C=3, meanwhile achieve efficient utilization of C4/C5 resources, which has very important research significance and industrial application value. The main technical problem of catalytic cracking of C=4 is how to obtain high selectivity of olefin products, especially the target product C=3 and to reduce non-olefin by-products, and its core lies in the development of high-efficiency catalysts. At present, the main industrial catalyst is modified ZSM-5. Titanium silicate molecular sieve TS-1 is a high-efficiency catalyst in the liquid phase ammoximation process of industrial cyclohexanone, which shows a typical Br{\o}nsted acid property after deactivation. Based on this, the deactivated TS-1 as an efficient catalyst for catalytic cracking of C=4 to produce C=3 was developed, and the result indicated that the deactivated TS-1 after acid treatment and potassium ion (K+) exchange could show the feature of high activity, high selectivity and high stability. Combined with nitric acid treating modification, K+ exchange experiment and the characterization techniques such as UV-Vis (UV-visible spectroscopy), FT-IR (Fourier transform infrared spectrometer) and NH3-TPD (temperature-programmed desorption of ammonia), it was found that the catalytic cracking active center of deactivated TS-1 is Br{\o}nsted acidic silyl hydroxyl group (Si-OH(Ti)) adjacent to the titanium hydroxyl group. The structure of this Br{\o}nsted acid site is completely different from the skeleton bridge Br{\o}nsted acid site (Si-(OH)-Al) of ZSM-5, meanwhile shows relatively weak acid strength. The unique acid property of Si-OH(Ti) could promote the main reaction path of catalytic cracking of C=4 to produce C=3 and inhibit the side reaction path of hydrogen transfer reaction. The discovery and application of the special Br{\o}nsted acid center of the deactivated TS-1 waste catalyst can provide a new idea for resource utilization of solid waste resources of spent catalyst.",

keywords = "Br{\o}nsted acid site, Catalyst, Catalyze, Deactivation, Hydrogen transfer reaction",

author = "Xin Huang and Yuxia Lin and Binghui Yan and Yueming Liu",

year = "2021",

month = oct,

doi = "10.11949/0438-1157.20210506",

language = "繁体中文",

volume = "72",

pages = "5183--5195",

journal = "Huagong Xuebao/CIESC Journal",

issn = "0438-1157",

publisher = "Materials China",

number = "10",

}

TY - JOUR

T1 - 失活TS-1高效催化C=4裂解制C=3反应的研究

AU - Huang, Xin

AU - Lin, Yuxia

AU - Yan, Binghui

AU - Liu, Yueming

PY - 2021/10

Y1 - 2021/10

N2 - Catalytic cracking of light olefins (C=4/C=5) can produce high value-added product C=3, meanwhile achieve efficient utilization of C4/C5 resources, which has very important research significance and industrial application value. The main technical problem of catalytic cracking of C=4 is how to obtain high selectivity of olefin products, especially the target product C=3 and to reduce non-olefin by-products, and its core lies in the development of high-efficiency catalysts. At present, the main industrial catalyst is modified ZSM-5. Titanium silicate molecular sieve TS-1 is a high-efficiency catalyst in the liquid phase ammoximation process of industrial cyclohexanone, which shows a typical Brønsted acid property after deactivation. Based on this, the deactivated TS-1 as an efficient catalyst for catalytic cracking of C=4 to produce C=3 was developed, and the result indicated that the deactivated TS-1 after acid treatment and potassium ion (K+) exchange could show the feature of high activity, high selectivity and high stability. Combined with nitric acid treating modification, K+ exchange experiment and the characterization techniques such as UV-Vis (UV-visible spectroscopy), FT-IR (Fourier transform infrared spectrometer) and NH3-TPD (temperature-programmed desorption of ammonia), it was found that the catalytic cracking active center of deactivated TS-1 is Brønsted acidic silyl hydroxyl group (Si-OH(Ti)) adjacent to the titanium hydroxyl group. The structure of this Brønsted acid site is completely different from the skeleton bridge Brønsted acid site (Si-(OH)-Al) of ZSM-5, meanwhile shows relatively weak acid strength. The unique acid property of Si-OH(Ti) could promote the main reaction path of catalytic cracking of C=4 to produce C=3 and inhibit the side reaction path of hydrogen transfer reaction. The discovery and application of the special Brønsted acid center of the deactivated TS-1 waste catalyst can provide a new idea for resource utilization of solid waste resources of spent catalyst.

AB - Catalytic cracking of light olefins (C=4/C=5) can produce high value-added product C=3, meanwhile achieve efficient utilization of C4/C5 resources, which has very important research significance and industrial application value. The main technical problem of catalytic cracking of C=4 is how to obtain high selectivity of olefin products, especially the target product C=3 and to reduce non-olefin by-products, and its core lies in the development of high-efficiency catalysts. At present, the main industrial catalyst is modified ZSM-5. Titanium silicate molecular sieve TS-1 is a high-efficiency catalyst in the liquid phase ammoximation process of industrial cyclohexanone, which shows a typical Brønsted acid property after deactivation. Based on this, the deactivated TS-1 as an efficient catalyst for catalytic cracking of C=4 to produce C=3 was developed, and the result indicated that the deactivated TS-1 after acid treatment and potassium ion (K+) exchange could show the feature of high activity, high selectivity and high stability. Combined with nitric acid treating modification, K+ exchange experiment and the characterization techniques such as UV-Vis (UV-visible spectroscopy), FT-IR (Fourier transform infrared spectrometer) and NH3-TPD (temperature-programmed desorption of ammonia), it was found that the catalytic cracking active center of deactivated TS-1 is Brønsted acidic silyl hydroxyl group (Si-OH(Ti)) adjacent to the titanium hydroxyl group. The structure of this Brønsted acid site is completely different from the skeleton bridge Brønsted acid site (Si-(OH)-Al) of ZSM-5, meanwhile shows relatively weak acid strength. The unique acid property of Si-OH(Ti) could promote the main reaction path of catalytic cracking of C=4 to produce C=3 and inhibit the side reaction path of hydrogen transfer reaction. The discovery and application of the special Brønsted acid center of the deactivated TS-1 waste catalyst can provide a new idea for resource utilization of solid waste resources of spent catalyst.

KW - Brønsted acid site

KW - Catalyst

KW - Catalyze

KW - Deactivation

KW - Hydrogen transfer reaction

UR - https://www.scopus.com/pages/publications/85117103471

U2 - 10.11949/0438-1157.20210506

DO - 10.11949/0438-1157.20210506

M3 - 文章

AN - SCOPUS:85117103471

SN - 0438-1157

VL - 72

SP - 5183

EP - 5195

JO - Huagong Xuebao/CIESC Journal

JF - Huagong Xuebao/CIESC Journal

IS - 10

ER -

失活TS-1高效催化C⁼₄裂解制C⁼₃反应的研究

Abstract

UN SDGs

Access to Document

Other files and links

Fingerprint

Cite this