Citation: Yan-Tong Xu, Zi-Ming Ye, De-Xuan Liu, Xiao-Yun Tian, Dong-Dong Zhou, Chun-Ting He, Xiao-Ming Chen. Non-3d metal modulated zinc imidazolate frameworks for CO₂ cycloaddition in simulated flue gas under ambient condition[J]. Chinese Chemical Letters, ;2023, 34(7): 107814. doi: 10.1016/j.cclet.2022.107814 shu

Non-3d metal modulated zinc imidazolate frameworks for CO₂ cycloaddition in simulated flue gas under ambient condition

Yan-Tong Xu ^{a, b, 1} ,
Zi-Ming Ye ^{a, 1} ,
De-Xuan Liu ^a ,
Xiao-Yun Tian ^a ,
Dong-Dong Zhou ^a ,
Chun-Ting He ^{a, c, *,} ,
Xiao-Ming Chen ^{a, *,}

a.
MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, Sun Yat-Sen University, Guangzhou 510275, China
b.
Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou 510640, China
c.
MOE Key Laboratory of Fluorine and Silicon for Energy Materials and Chemistry, College of Chemistry and Chemical Engineering, Jiangxi Normal University, Nanchang 330022, China

hct@jxnu.edu.cn

cxm@mail.sysu.edu.cn

Received Date: 29 July 2022
Revised Date: 31 August 2022
Accepted Date: 6 September 2022
Available Online: 11 September 2022

Figures(5)

Cycloaddition of CO₂ and epoxide into cyclic carbonate is one of the most efficient ways for CO₂ conversion with 100% atom-utilization. Metal–organic frameworks are a kind of potential heterogeneous catalysts, however, high temperature, high pressure, and high-purity CO₂ are still required for the reaction. Here, we report two new Zn(Ⅱ) imidazolate frameworks incoporating MoO₄^2– or WO₄^2– units, which can catalyse cycloaddition of CO₂ and epichlorohydrin at room temperature and atomospheric pressure, giving 95% yield after 24 h in pure CO₂ and 98% yield after 48 h in simulated flue gas (15% CO₂ + 85% N₂), respectively. For comparison, the analogic Zn(Ⅱ) imidazolate framework MAF-6 without non-3d metal oxide units showed 71% and 33% yields under the same conditions, respectively. The insightful modulation mechanisms of the MoO₄^2– unit in optimizing the electronic structure of Zn(Ⅱ) centre, facilitating the rate-determined ring opening process, and minimizing the reaction activation energy, were revealed by X-ray photoelectron spectroscopy, temperature programmed desorption and computational calculations.
- Non-3d metal modulation,
- Metal-organic framework,
- CO₂ fixation,
- Flue gas,
- Cycloaddition reaction
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Non-3d metal modulated zinc imidazolate frameworks for CO2 cycloaddition in simulated flue gas under ambient condition

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Non-3d metal modulated zinc imidazolate frameworks for CO₂ cycloaddition in simulated flue gas under ambient condition