Citation: Yanhong Chen, Haiyan An, Shenzhen Chang, Yanqin Li, Tieqi Xu, Qingshan Zhu, Huiyun Luo, Yaohui Huang, Yuting Wei. Two pseudo-polymorphic porous POM-pillared MOFs for sulfide-sulfoxide transformation: Efficient synergistic effects of POM precursors, metal sites and microstructures[J]. Chinese Chemical Letters, ;2023, 34(7): 107856. doi: 10.1016/j.cclet.2022.107856 shu

Two pseudo-polymorphic porous POM-pillared MOFs for sulfide-sulfoxide transformation: Efficient synergistic effects of POM precursors, metal sites and microstructures

School of Chemical Engineering, Dalian University of Technology, Dalian 116023, China

anhy@dlut.edu.cn

tqxu@dlut.edu.cn

Received Date: 21 July 2022
Revised Date: 16 August 2022
Accepted Date: 22 September 2022
Available Online: 27 September 2022

Figures(5)

Developing sustainable and powerful heterogeneous catalytic systems to convert sulfides into high-value sulfoxide products has become a particularly appealing field and an arduous challenge. In this work, two porous polyoxometalate-pillared metal-organic frameworks, formulated as H_3n[Cu₃(pidc)₂(H₂O)_2.5]₂[PW₁₂O₄₀]_n·xH₂O (n = 1.5, x = 6 for 1, n = 1, x = 12 for 2; and H₃pidc = 2-(3-pyridinyl)-1H-imidazole-4,5-dicarboxylic acid), were consciously manufacture and employed for heterogeneously catalyzed sulfide-sulfoxide transformation. Structural analysis shows that 1 and 2 exhibit similar porous frameworks with nearly identical two-dimensional metal-organic layers further pillared by tetradentate POM ligands with different coordination modes, which also result in the porosity of 1 being almost twice that of 2. In catalyzing the conversion of methyl phenyl sulfide (MPS) to methyl phenyl sulfoxide (MPSO), 1 can convert nearly 100% of MPS into MPSO within 30 min, while 2 achieved the similar results requires 50 min. The higher activity of 1 may be attributed to its larger channel that can provide more active sites and more efficient mass transfer process. Systematic structure-activity analyses and mechanistic studies revealed dual-reaction pathways driven by POM sites and metal sites assisted by the structural microenvironment.
- Polyoxometalate,
- Porous frameworks,
- POMOF,
- Heterogeneous catalysis,
- Sulfide oxidation
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