Heterogeneity of polyoxometalates by confining within ordered mesopores: Toward efficient oxidation of benzene to phenol

Yan Leng; Yuchen Jiang; Honggeng Peng; Zihao Zhang; Miaomiao Liu; Kecheng Jie; Pengfei Zhang; Sheng Dai

doi:10.1039/c9cy00288j

Heterogeneity of polyoxometalates by confining within ordered mesopores: Toward efficient oxidation of benzene to phenol

Yan Leng, Yuchen Jiang, Honggeng Peng, Zihao Zhang, Miaomiao Liu, Kecheng Jie, Pengfei Zhang, Sheng Dai

Nanomaterials Chemistry Group

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

12 Scopus citations

Abstract

Polyoxometalates (POMs) are a family of promising homogeneous catalysts for various processes. The design of POM-based heterogeneous catalysts, while important for real-world catalysis, is an important topic. Herein, a green and effective mechanochemical assembly strategy was developed to encapsulate the POM inside the ordered mesoporous polymer (OMP) with biomass tannin as the precursor. The strategy was realized by solid-state ball milling of the POM, using 3-aminophenol and tannin with F127 as the template, and removing the template by calcination. The POM-containing materials possessed uniform mesopores (5-10 nm) and high surface areas (150-250 m² g^-1). In particular, the H₅PM₁₀V₂O₄₀-based OMP exhibited good activity (33% conversion and 100% selectivity) and stability (reused in five runs) for the hydroxylation of benzene to phenol. The results of experiments and characterizations demonstrated that the unique confinement structure and the reversible V⁵⁺/V⁴⁺ redox pairs induced by the strong interaction between the OMP and PMoV may account for the good catalytic performance.

Original language	English
Pages (from-to)	2173-2179
Number of pages	7
Journal	Catalysis Science and Technology
Volume	9
Issue number	9
DOIs	https://doi.org/10.1039/c9cy00288j
State	Published - 2019

Funding

This research was sponsored by the U.S. Department of Energy, Office of Basic Energy Sciences, Chemical Sciences, Geoscience, and Bioscience Division (ZZ, ML, KJ, SD). YL and YJ thank the Jiangsu Key Laboratory for Biomass Energy and Material Open Fund Project (JSBEM201906) and MOE & SAFEA for the 111 Project (No. B13025). P. F. Z. acknowledges the Shanghai Pujiang Program (Grant No. 17PJ1403500), the Thousand Talent Program, and the National Natural Science Foundation of China (Grant No. 21776174) for support.

Funders	Funder number
Bioscience Division
Jiangsu Key Laboratory for Biomass Energy and Material Open Fund	JSBEM201906
Office of Basic Energy Sciences
Shanghai Pujiang Program	17PJ1403500
U.S. Department of Energy
National Natural Science Foundation of China	21776174
National Natural Science Foundation of China
Ministry of Education of the People's Republic of China
State Administration of Foreign Experts Affairs
Higher Education Discipline Innovation Project

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title = "Heterogeneity of polyoxometalates by confining within ordered mesopores: Toward efficient oxidation of benzene to phenol",

abstract = "Polyoxometalates (POMs) are a family of promising homogeneous catalysts for various processes. The design of POM-based heterogeneous catalysts, while important for real-world catalysis, is an important topic. Herein, a green and effective mechanochemical assembly strategy was developed to encapsulate the POM inside the ordered mesoporous polymer (OMP) with biomass tannin as the precursor. The strategy was realized by solid-state ball milling of the POM, using 3-aminophenol and tannin with F127 as the template, and removing the template by calcination. The POM-containing materials possessed uniform mesopores (5-10 nm) and high surface areas (150-250 m2 g-1). In particular, the H5PM10V2O40-based OMP exhibited good activity (33% conversion and 100% selectivity) and stability (reused in five runs) for the hydroxylation of benzene to phenol. The results of experiments and characterizations demonstrated that the unique confinement structure and the reversible V5+/V4+ redox pairs induced by the strong interaction between the OMP and PMoV may account for the good catalytic performance.",

author = "Yan Leng and Yuchen Jiang and Honggeng Peng and Zihao Zhang and Miaomiao Liu and Kecheng Jie and Pengfei Zhang and Sheng Dai",

note = "Publisher Copyright: {\textcopyright} 2019 The Royal Society of Chemistry.",

year = "2019",

doi = "10.1039/c9cy00288j",

language = "English",

volume = "9",

pages = "2173--2179",

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TY - JOUR

T1 - Heterogeneity of polyoxometalates by confining within ordered mesopores

T2 - Toward efficient oxidation of benzene to phenol

AU - Leng, Yan

AU - Jiang, Yuchen

AU - Peng, Honggeng

AU - Zhang, Zihao

AU - Liu, Miaomiao

AU - Jie, Kecheng

AU - Zhang, Pengfei

AU - Dai, Sheng

PY - 2019

Y1 - 2019

N2 - Polyoxometalates (POMs) are a family of promising homogeneous catalysts for various processes. The design of POM-based heterogeneous catalysts, while important for real-world catalysis, is an important topic. Herein, a green and effective mechanochemical assembly strategy was developed to encapsulate the POM inside the ordered mesoporous polymer (OMP) with biomass tannin as the precursor. The strategy was realized by solid-state ball milling of the POM, using 3-aminophenol and tannin with F127 as the template, and removing the template by calcination. The POM-containing materials possessed uniform mesopores (5-10 nm) and high surface areas (150-250 m2 g-1). In particular, the H5PM10V2O40-based OMP exhibited good activity (33% conversion and 100% selectivity) and stability (reused in five runs) for the hydroxylation of benzene to phenol. The results of experiments and characterizations demonstrated that the unique confinement structure and the reversible V5+/V4+ redox pairs induced by the strong interaction between the OMP and PMoV may account for the good catalytic performance.

AB - Polyoxometalates (POMs) are a family of promising homogeneous catalysts for various processes. The design of POM-based heterogeneous catalysts, while important for real-world catalysis, is an important topic. Herein, a green and effective mechanochemical assembly strategy was developed to encapsulate the POM inside the ordered mesoporous polymer (OMP) with biomass tannin as the precursor. The strategy was realized by solid-state ball milling of the POM, using 3-aminophenol and tannin with F127 as the template, and removing the template by calcination. The POM-containing materials possessed uniform mesopores (5-10 nm) and high surface areas (150-250 m2 g-1). In particular, the H5PM10V2O40-based OMP exhibited good activity (33% conversion and 100% selectivity) and stability (reused in five runs) for the hydroxylation of benzene to phenol. The results of experiments and characterizations demonstrated that the unique confinement structure and the reversible V5+/V4+ redox pairs induced by the strong interaction between the OMP and PMoV may account for the good catalytic performance.

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Heterogeneity of polyoxometalates by confining within ordered mesopores: Toward efficient oxidation of benzene to phenol

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