Well-Arranged Hollow Au@Zn/Ni-MOF-2-NH2Core-Shell Nanocatalyst with Enhanced Catalytic Activity for Biomass-Derived d -Xylose Oxidation

Nianqiao Qin; Xiaoyan Wu; Xinxin Liu; Zhong Hua Xue; Mohd Muddassir; Hiroshi Sakiyama; Chi Xia; Chunyan Zhang; Linghui Zhu; Fei Ke

doi:10.1021/acssuschemeng.1c07977

Well-Arranged Hollow Au@Zn/Ni-MOF-2-NH₂Core-Shell Nanocatalyst with Enhanced Catalytic Activity for Biomass-Derived d -Xylose Oxidation

Nianqiao Qin, Xiaoyan Wu, Xinxin Liu, Zhong Hua Xue^*, Mohd Muddassir, Hiroshi Sakiyama, Chi Xia, Chunyan Zhang, Linghui Zhu, Fei Ke^*

^*Corresponding author for this work

Advanced Membranes and Porous Materials Center

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

12 Scopus citations

Abstract

Highly base-free catalytic of biomass-derived feedstock into value-added chemical is of great interest in catalysis but remains a challenge. Herein, a hollow nanocatalyst composed of Au nanoparticles as the core and Zn/Ni bimetallic metal-organic frameworks (MOFs) functionalized with the -NH2 ligand as the shell (Au@Zn/Ni-MOF-2-NH2) is fabricated through a straightforward one-pot hydrothermal method for a highly efficient, selective, and base-free synthesis of d-xylonic acid by the catalytic oxidation of d-xylose. Experimental and theoretical results confirmed the key role of hollow core-shell Au@Zn/Ni-MOF-2-NH2 in providing in-depth synergistic effects between the Au nanoparticles and the porous MOF and further facilitating the transport of reactant and product molecules, triggering a noticeably impressive turnover frequency value of 76.53 h-1 for d-xylonic acid generation, outperforming the bare Au nanocatalyst by 306 times. The highly integrated structure of Au@Zn/Ni-MOF-2-NH2 is stable for recycled use during the oxidation process, which further demonstrates the superior availability of such a bimetallic MOF-based hollow core-shell heterogeneous nanocatalyst.

Original language	English (US)
Pages (from-to)	5396-5403
Number of pages	8
Journal	ACS Sustainable Chemistry and Engineering
Volume	10
Issue number	17
DOIs	https://doi.org/10.1021/acssuschemeng.1c07977
State	Published - May 2 2022

Bibliographical note

Funding Information:
The authors gratefully acknowledge the funding support from the National Natural Science Foundation of China (NSFC, 21501003), the Program for Excellent Talents in the University of the Ministry of Education of China (gxyqZD2020008), the Open Fund of State Key Laboratory of Tea Plant Biology and Utilization (SKLTOF20190116), the National Undergraduate Training Programs for Innovation and Entrepreneurship of Anhui Agriculture University (202010364041), and Researchers Supporting Project number (RSP-2021/141), King Saud University, Riyadh, Saudi Arabia.

Publisher Copyright:
© 2022 American Chemical Society.

Keywords

core-shell
d-xylose oxidation
density functional theory
hollow nanostructure
metal-organic frameworks

ASJC Scopus subject areas

General Chemistry
Environmental Chemistry
General Chemical Engineering
Renewable Energy, Sustainability and the Environment

UN SDGs

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

Access to Document

10.1021/acssuschemeng.1c07977

Cite this

@article{b5a425136aeb4fdba0c0e62c686e157d,

title = "Well-Arranged Hollow Au@Zn/Ni-MOF-2-NH2Core-Shell Nanocatalyst with Enhanced Catalytic Activity for Biomass-Derived d -Xylose Oxidation",

abstract = "Highly base-free catalytic of biomass-derived feedstock into value-added chemical is of great interest in catalysis but remains a challenge. Herein, a hollow nanocatalyst composed of Au nanoparticles as the core and Zn/Ni bimetallic metal-organic frameworks (MOFs) functionalized with the -NH2 ligand as the shell (Au@Zn/Ni-MOF-2-NH2) is fabricated through a straightforward one-pot hydrothermal method for a highly efficient, selective, and base-free synthesis of d-xylonic acid by the catalytic oxidation of d-xylose. Experimental and theoretical results confirmed the key role of hollow core-shell Au@Zn/Ni-MOF-2-NH2 in providing in-depth synergistic effects between the Au nanoparticles and the porous MOF and further facilitating the transport of reactant and product molecules, triggering a noticeably impressive turnover frequency value of 76.53 h-1 for d-xylonic acid generation, outperforming the bare Au nanocatalyst by 306 times. The highly integrated structure of Au@Zn/Ni-MOF-2-NH2 is stable for recycled use during the oxidation process, which further demonstrates the superior availability of such a bimetallic MOF-based hollow core-shell heterogeneous nanocatalyst.",

keywords = "core-shell, d-xylose oxidation, density functional theory, hollow nanostructure, metal-organic frameworks",

author = "Nianqiao Qin and Xiaoyan Wu and Xinxin Liu and Xue, {Zhong Hua} and Mohd Muddassir and Hiroshi Sakiyama and Chi Xia and Chunyan Zhang and Linghui Zhu and Fei Ke",

note = "Funding Information: The authors gratefully acknowledge the funding support from the National Natural Science Foundation of China (NSFC, 21501003), the Program for Excellent Talents in the University of the Ministry of Education of China (gxyqZD2020008), the Open Fund of State Key Laboratory of Tea Plant Biology and Utilization (SKLTOF20190116), the National Undergraduate Training Programs for Innovation and Entrepreneurship of Anhui Agriculture University (202010364041), and Researchers Supporting Project number (RSP-2021/141), King Saud University, Riyadh, Saudi Arabia. Publisher Copyright: {\textcopyright} 2022 American Chemical Society.",

year = "2022",

month = may,

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doi = "10.1021/acssuschemeng.1c07977",

language = "English (US)",

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T1 - Well-Arranged Hollow Au@Zn/Ni-MOF-2-NH2Core-Shell Nanocatalyst with Enhanced Catalytic Activity for Biomass-Derived d -Xylose Oxidation

AU - Qin, Nianqiao

AU - Wu, Xiaoyan

AU - Liu, Xinxin

AU - Xue, Zhong Hua

AU - Muddassir, Mohd

AU - Sakiyama, Hiroshi

AU - Xia, Chi

AU - Zhang, Chunyan

AU - Zhu, Linghui

AU - Ke, Fei

N1 - Funding Information: The authors gratefully acknowledge the funding support from the National Natural Science Foundation of China (NSFC, 21501003), the Program for Excellent Talents in the University of the Ministry of Education of China (gxyqZD2020008), the Open Fund of State Key Laboratory of Tea Plant Biology and Utilization (SKLTOF20190116), the National Undergraduate Training Programs for Innovation and Entrepreneurship of Anhui Agriculture University (202010364041), and Researchers Supporting Project number (RSP-2021/141), King Saud University, Riyadh, Saudi Arabia. Publisher Copyright: © 2022 American Chemical Society.

PY - 2022/5/2

Y1 - 2022/5/2

N2 - Highly base-free catalytic of biomass-derived feedstock into value-added chemical is of great interest in catalysis but remains a challenge. Herein, a hollow nanocatalyst composed of Au nanoparticles as the core and Zn/Ni bimetallic metal-organic frameworks (MOFs) functionalized with the -NH2 ligand as the shell (Au@Zn/Ni-MOF-2-NH2) is fabricated through a straightforward one-pot hydrothermal method for a highly efficient, selective, and base-free synthesis of d-xylonic acid by the catalytic oxidation of d-xylose. Experimental and theoretical results confirmed the key role of hollow core-shell Au@Zn/Ni-MOF-2-NH2 in providing in-depth synergistic effects between the Au nanoparticles and the porous MOF and further facilitating the transport of reactant and product molecules, triggering a noticeably impressive turnover frequency value of 76.53 h-1 for d-xylonic acid generation, outperforming the bare Au nanocatalyst by 306 times. The highly integrated structure of Au@Zn/Ni-MOF-2-NH2 is stable for recycled use during the oxidation process, which further demonstrates the superior availability of such a bimetallic MOF-based hollow core-shell heterogeneous nanocatalyst.

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