General Synthesis of Ordered Mesoporous Carbonaceous Hybrid Nanostructures with Molecularly Dispersed Polyoxometallates

Chunhong Chen; Shanjun Mao; Chaoliang Tan; Zhe Wang; Yiyao Ge; Qinglang Ma; Xiao Zhang; Guodong Qi; Jun Xu; Zhanxi Fan; Yong Wang

doi:10.1002/anie.202104028

General Synthesis of Ordered Mesoporous Carbonaceous Hybrid Nanostructures with Molecularly Dispersed Polyoxometallates

Angew Chem Int Ed Engl. 2021 Jul 5;60(28):15556-15562. doi: 10.1002/anie.202104028. Epub 2021 Jun 7.

Authors

Chunhong Chen^{1

2}, Shanjun Mao¹, Chaoliang Tan³, Zhe Wang¹, Yiyao Ge², Qinglang Ma², Xiao Zhang², Guodong Qi⁴, Jun Xu⁴, Zhanxi Fan⁵, Yong Wang^{1

6}

Affiliations

¹ Advanced Materials and Catalysis Group, Institute of Catalysis, Department of Chemistry, Zhejiang University, Hangzhou, 310028, P. R. China.
² Center for Programmable Materials, School of Materials Science and Engineering, Nanyang Technological University, 50 Nanyang Avenue, Singapore, 639798, Singapore.
³ Department of Electrical Engineering, City University of Hong Kong, 83 Tat Chee Avenue, Kowloon, Hong Kong, China.
⁴ National Centre for Magnetic Resonance in Wuhan, State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, Wuhan Institute of Physics and Mathematics, Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences, Wuhan, 430071, P. R. China.
⁵ Department of Chemistry, City University of Hong Kong, 83 Tat Chee Avenue, Kowloon, Hong Kong, China.
⁶ College of Chemistry and Molecular Engineering, Zhengzhou University, Zhengzhou, 450001, China.

PMID: 33942452
DOI: 10.1002/anie.202104028

Abstract

Hybrid nanomaterials with controlled dimensions, intriguing components and ordered structures have attracted significant attention in nanoscience and technology. Herein, we report a facile and green polyoxometallate (POM)-assisted hydrothermal carbonization strategy for synthesis of carbonaceous hybrid nanomaterials with molecularly dispersed POMs and ordered mesopores. By using various polyoxometallates such as ammonium phosphomolybdate, silicotungstic acid, and phosphotungstic acid, our approach can be generalized to synthesize ordered mesoporous hybrid nanostructures with diverse compositions and morphologies (nanosheet-assembled hierarchical architectures, nanospheres, and nanorods). Moreover, the ordered mesoporous nanosheet-assembled hierarchical hybrids with molecularly dispersed POMs exhibit remarkable catalytic activity toward the dehydration of tert-butanol with the high isobutene selectivity (100 %) and long-term catalytic durability (80 h).

Keywords: biomass; hydrothermal carbonization; molecularly dispersed polyoxometalates; ordered mesopore; single-molecule heterogeneous catalyst.

Abstract

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