Enhanced catalytic oxidation performance of K+-modified Ti-MWW through selective breaking of interfacial hydrogen-bonding interactions of H2O2

Yunkai Yu; Zhimou Tang; Wei Liu; Jia Wang; Zhen Chen; Kaixu Shen; Rui Wang; Haoxin Liu; Xin Huang; Yueming Liu

doi:10.1016/j.apcata.2019.117270

Enhanced catalytic oxidation performance of K⁺-modified Ti-MWW through selective breaking of interfacial hydrogen-bonding interactions of H₂O₂

Yunkai Yu, Zhimou Tang, Wei Liu, Jia Wang, Zhen Chen, Kaixu Shen, Rui Wang, Haoxin Liu, Xin Huang, Yueming Liu

School of Chemistry and Molecular Engineering

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

15 Scopus citations

Abstract

Cationic modification was applied to Ti-MWW zeolite via the treatment of potassium chloride (KCl). Compared to the original Ti-MWW zeolite, the K-modified Ti-MWW sample (Ti-MWW-K) exhibited much improved catalytic activity, selectivity and stability in the liquid-phase epoxidation of alkenes. Our investigation shows that the K⁺ modification has negligible effect on the physicochemical properties, the state of the Ti active sites and the Lewis acidic strength of the Ti-MWW catalyst. Our result has further indicated that breaking of the hydrogen-bonding interactions between the O_β atom of H₂O₂ (H_α-O_α-O_β-H_end) and the H atom of the silanols adjacent to the Ti-OH (Si[sbnd]OH(HO[sbnd]Ti)) in the Ti-MWW-K zeolite promotes the activation of H₂O₂, which is responsible for its superior catalytic oxidation activity. This finding helps shed light on utilizing the hydrogen-bonding interactions based on the titanosilicates/H₂O₂ system to achieve the excellent catalytic oxidation performance.

Original language	English
Article number	117270
Journal	Applied Catalysis A: General
Volume	587
DOIs	https://doi.org/10.1016/j.apcata.2019.117270
State	Published - 25 Oct 2019

Keywords

Activation
Cationic modification
Hydrogen-bonding interactions
Oxidation
Silanols
Titanosilicates

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10.1016/j.apcata.2019.117270

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@article{3ad0917780ba446093b91a1bfa781fd6,

title = "Enhanced catalytic oxidation performance of K+-modified Ti-MWW through selective breaking of interfacial hydrogen-bonding interactions of H2O2",

abstract = "Cationic modification was applied to Ti-MWW zeolite via the treatment of potassium chloride (KCl). Compared to the original Ti-MWW zeolite, the K-modified Ti-MWW sample (Ti-MWW-K) exhibited much improved catalytic activity, selectivity and stability in the liquid-phase epoxidation of alkenes. Our investigation shows that the K+ modification has negligible effect on the physicochemical properties, the state of the Ti active sites and the Lewis acidic strength of the Ti-MWW catalyst. Our result has further indicated that breaking of the hydrogen-bonding interactions between the Oβ atom of H2O2 (Hα-Oα-Oβ-Hend) and the H atom of the silanols adjacent to the Ti-OH (Si[sbnd]OH(HO[sbnd]Ti)) in the Ti-MWW-K zeolite promotes the activation of H2O2, which is responsible for its superior catalytic oxidation activity. This finding helps shed light on utilizing the hydrogen-bonding interactions based on the titanosilicates/H2O2 system to achieve the excellent catalytic oxidation performance.",

keywords = "Activation, Cationic modification, Hydrogen-bonding interactions, Oxidation, Silanols, Titanosilicates",

author = "Yunkai Yu and Zhimou Tang and Wei Liu and Jia Wang and Zhen Chen and Kaixu Shen and Rui Wang and Haoxin Liu and Xin Huang and Yueming Liu",

note = "Publisher Copyright: {\textcopyright} 2019 Elsevier B.V.",

year = "2019",

month = oct,

day = "25",

doi = "10.1016/j.apcata.2019.117270",

language = "英语",

volume = "587",

journal = "Applied Catalysis A: General",

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TY - JOUR

T1 - Enhanced catalytic oxidation performance of K+-modified Ti-MWW through selective breaking of interfacial hydrogen-bonding interactions of H2O2

AU - Yu, Yunkai

AU - Tang, Zhimou

AU - Liu, Wei

AU - Wang, Jia

AU - Chen, Zhen

AU - Shen, Kaixu

AU - Wang, Rui

AU - Liu, Haoxin

AU - Huang, Xin

AU - Liu, Yueming

PY - 2019/10/25

Y1 - 2019/10/25

N2 - Cationic modification was applied to Ti-MWW zeolite via the treatment of potassium chloride (KCl). Compared to the original Ti-MWW zeolite, the K-modified Ti-MWW sample (Ti-MWW-K) exhibited much improved catalytic activity, selectivity and stability in the liquid-phase epoxidation of alkenes. Our investigation shows that the K+ modification has negligible effect on the physicochemical properties, the state of the Ti active sites and the Lewis acidic strength of the Ti-MWW catalyst. Our result has further indicated that breaking of the hydrogen-bonding interactions between the Oβ atom of H2O2 (Hα-Oα-Oβ-Hend) and the H atom of the silanols adjacent to the Ti-OH (Si[sbnd]OH(HO[sbnd]Ti)) in the Ti-MWW-K zeolite promotes the activation of H2O2, which is responsible for its superior catalytic oxidation activity. This finding helps shed light on utilizing the hydrogen-bonding interactions based on the titanosilicates/H2O2 system to achieve the excellent catalytic oxidation performance.

AB - Cationic modification was applied to Ti-MWW zeolite via the treatment of potassium chloride (KCl). Compared to the original Ti-MWW zeolite, the K-modified Ti-MWW sample (Ti-MWW-K) exhibited much improved catalytic activity, selectivity and stability in the liquid-phase epoxidation of alkenes. Our investigation shows that the K+ modification has negligible effect on the physicochemical properties, the state of the Ti active sites and the Lewis acidic strength of the Ti-MWW catalyst. Our result has further indicated that breaking of the hydrogen-bonding interactions between the Oβ atom of H2O2 (Hα-Oα-Oβ-Hend) and the H atom of the silanols adjacent to the Ti-OH (Si[sbnd]OH(HO[sbnd]Ti)) in the Ti-MWW-K zeolite promotes the activation of H2O2, which is responsible for its superior catalytic oxidation activity. This finding helps shed light on utilizing the hydrogen-bonding interactions based on the titanosilicates/H2O2 system to achieve the excellent catalytic oxidation performance.

KW - Activation

KW - Cationic modification

KW - Hydrogen-bonding interactions

KW - Oxidation

KW - Silanols

KW - Titanosilicates

UR - https://www.scopus.com/pages/publications/85072693359

U2 - 10.1016/j.apcata.2019.117270

DO - 10.1016/j.apcata.2019.117270

M3 - 文章

AN - SCOPUS:85072693359

SN - 0926-860X

VL - 587

JO - Applied Catalysis A: General

JF - Applied Catalysis A: General

M1 - 117270

ER -

Enhanced catalytic oxidation performance of K⁺-modified Ti-MWW through selective breaking of interfacial hydrogen-bonding interactions of H₂O₂

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Keywords

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