Robust Fluorine-Decorated {Yb 4 }-Organic Framework for C 2 H 6 Capture and Efficient Catalytic Performance on CO 2 -Epoxide Cycloaddition

• Published in: ACS applied materials & interfaces Vol. 17; no. 20; pp. 29788 - 29798
• Main Authors: Wang, Zhen-Feng, Fei, Yang, Qin, Aimiao, Zhang, Shuhua, Zhang, Xiutang
• Format: Journal Article
• Language: English
• Published: United States 21.05.2025
• Subjects: chemical fixation of CO2; ytterbium(III)-organic; fluorine group; adsorption capacity
• ISSN: 1944-8244; 1944-8252
• DOI: 10.1021/acsami.5c07205

Fluorine-functionalized MOFs have excellent unusual properties such as gas adsorption and separation and catalysis, but the functionalization of existing ligands and the self-assembly of functionalized MOFs remain a challenge. Herein, we report a robust fluorine-functionalized nanochannel-based ytterbium(III)-organic framework of {(Me NH )[Yb (CFPDA) (μ -HCO )(μ -OH) (H O) ]·4DMF·5H O} ( , H CFPDA = 4,4'-(4-(4-carboxy-2-fluorophenyl)pyridine-2,6-diyl)diisophthalic acid) with [Yb (μ -OH) (μ -HCO )(H O) ] clusters as secondary building units (SBUs). Compared to reported anionic skeleton of [Yb (BDCP) (μ -HCO )(μ -OH) (H O) ] ( ), the void volume of (54.1%) is slightly lower than that of (56.7%), which is caused by functionalized fluorine atoms on the ligand of H BDCP. Because of the introduction of fluorine groups, activated displays a higher adsorption capacity for CO along with the value of 117.5 cm /g (273 K) and 63.1 cm /g (298 K). Further, activated has a high ethane (C H ) separation performance over the mixture of C H /C H with the selectivity of 1.6, enabling the purity of recycled C H to reach 99.99%. Moreover, the CO -epoxide cycloaddition could be efficiently catalyzed by under comparatively mild conditions. Under optimal catalytic conditions of 0.13 mol % MOFs, 1.69 mol % -Bu NBr, 0.7 MPa CO , 70 °C, and 3 h, the conversion yield of SO to SC catalyzed by is 26% higher than that catalyzed by . The excellent separation and catalytic performance should be attributed to the combined diverse functional groups such as Lewis acidic sites of Yb , Lewis basic sites of -F and N atoms, and electrophilic H-bond donors (HBD) of μ -OH and μ -HCO moieties. Hence, this work not only reports a fluorine-functionalized multifunctional material but also provides an in-depth insight into the synthetic strategy of functionalized metal-organic host frameworks.