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A Stable Zn-Based Metal–Organic Framework as an Efficient Catalyst for Carbon Dioxide Cycloaddition and Alcoholysis at Mild Conditions

  • Zhiqiang Luo
  • Jun WangEmail author
  • Yanqing He
  • Qiong Ao
  • Qiang Deng
  • Zheling Zeng
  • Hongming Wang
  • Shuguang DengEmail author
Article
  • 43 Downloads

Abstract

Developing highly efficient heterogeneous catalysts for cycloaddition of CO2 and epoxides to produce cyclic carbonates is promising but challenging. In this work, a novel three-dimensional metal organic framework (MOF) with cylinder pore systems and unsaturated Zn sites has been demonstrated as potent candidate in CO2 fixation at mild and solvent-free conditions. The Zn(atz)(bdc)0.5, where atz = aminotriazole and H2bdc = terephthalic, exhibits microporous nature that can regulate the catalytic interaction of active centers and substrates. The structure stability has been systematically investigated and proven to be sufficient for practical application. Furthermore, the cooperative effects of porosity, CO2 binding affinity, activation centers, and synergism with co-catalyst have been deeply investigated. Moreover, high propylene epoxide conversion (97%) and selectivity (> 99%) have been achieved at mild conditions (60 °C and 1 MPa) with excellent cycle stability. Owing to the well-defined pore system, an obvious substrates selectivity has been clearly observed. A possible catalytic mechanism has been proposed and verified by DFT calculations. Furthermore, the prepared Zn-MOF can also be used as an efficient heterogeneous catalyst for the reaction of epoxides with alcohols to produce β-alkoxy alcohol.

Graphic Abstract

Keywords

Metal organic frameworks Cycloaddition CO2 conversion Alcoholysis 

Notes

Acknowledgements

This research work is partially supported by the National Natural Science Foundation of China (No.51672186 and 21908090), Natural Science Foundation of Jiangxi Province (No.20192ACB21015), and the start-up funds of Nanchang University and Arizona State University.

Compliance with Ethical Standards

Conflict of interest

The authors declare that they have no conflict of interests.

Supplementary material

10562_2019_3053_MOESM1_ESM.doc (2.7 mb)
Supplementary material 1 (DOC 2782 kb)

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Copyright information

© Springer Science+Business Media, LLC, part of Springer Nature 2019

Authors and Affiliations

  1. 1.Key Laboratory of Poyang Environment and Resource Utilization (Nanchang University)Ministry of EducationNanchangPeople’s Republic of China
  2. 2.School of Resource Environmental and Chemical EngineeringNanchang UniversityNanchangPeople’s Republic of China
  3. 3.Institute for Advanced StudyNanchang UniversityNanchangChina
  4. 4.School for Engineering of Matter, Transport and EnergyArizona State UniversityTempeUSA

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