Citation: Longlong Geng, Huiling Liu, Wenfeng Zhou, Yong-Zheng Zhang, Hongliang Huang, Da-Shuai Zhang, Hui Hu, Chao Lv, Xiuling Zhang, Suijun Liu. Construction of metal-organic frameworks with unsaturated Cu sites for efficient and fast reduction of nitroaromatics: A combined experimental and theoretical study[J]. Chinese Chemical Letters, ;2024, 35(8): 109120. doi: 10.1016/j.cclet.2023.109120 shu

Construction of metal-organic frameworks with unsaturated Cu sites for efficient and fast reduction of nitroaromatics: A combined experimental and theoretical study

Longlong Geng ^{a, b} ,
Huiling Liu ^a ,
Wenfeng Zhou ^{a, b} ,
Yong-Zheng Zhang ^{a, *,} ,
Hongliang Huang ^c ,
Da-Shuai Zhang ^{a, b, *,} ,
Hui Hu ^a ,
Chao Lv ^a ,
Xiuling Zhang ^{a, b} ,
Suijun Liu ^{d, *,}

a.
Shandong Provincial Key Laboratory of Monocrystalline Silicon Semiconductor Materials and Technology, College of Chemistry and Chemical Engineering, Dezhou University, Dezhou 253023, China
b.
School of Chemistry and Chemical Engineering, Shandong University of Technology, Zibo 255000, China
c.
State Key Laboratory of Separation Membranes and Membrane Processes, School of Chemical Engineering and Technology, Tiangong University, Tianjin 300387, China
d.
School of Chemistry and Chemical Engineering, Jiangxi Provincial Key Laboratory of Functional Molecular Materials Chemistry, Jiangxi University of Science and Technology, Ganzhou 341000, China

zhangyongzheng23@163.com

dashuai_74@163.com

sjliu@jxust.edu.cn

Received Date: 8 August 2023
Revised Date: 6 September 2023
Accepted Date: 18 September 2023
Available Online: 20 September 2023

Figures(5)

Metal-organic frameworks (MOFs) functionalized with open metal sites (OMSs) have received widespread attention in various applications due to their fascinating electronic properties and unique interactions with guest molecules. However, rational tailoring of the coordination environment of metal nodes during the synthesis of MOFs remains a great challenge due to their tendency of saturated coordination with linkers. Herein, we reported the construction of three new MOFs featuring unsaturated Cu(Ⅱ) sites, namely [Cu(HCOO)(pzta)]_n (HL-1), {[Cu(PTA)_0.5(pzta)(H₂O)]·2H₂O}_n (HL-2) and [Cu(NA)_0.5(pzta)]_n (HL-3) (Hpzta = 3-pyrazinyl-1,2,4-triazole; PTA = terephthalic acid; NA = 1,4-naphthalene dicarboxylic acid), based on the mixed-linker strategy via specific selection of versatile Hpzta ligand and carboxylate ligands. Remarkably, the obtained MOFs exhibited excellent activity and good recyclability for the catalytic reduction of nitroaromatics under mild conditions (25 ℃ and 1 atm). In particular, the complete conversion of 4-nitrophenol (4-NP) took only 30 s on HL-2, reaching a record-high TOF value compared with previously reported metal catalysts. The combined experimental and theoretical studies on HL-2 revealed that the open Cu site with positive-charged nature could improve the adsorption and subsequent electron transport between the substrates, and was responsible for the outstanding performance. This work shined lights on the further enhancement of performance for MOFs through rational OMSs construction.
- Metal-organic frameworks,
- Open metal sites,
- Catalysis,
- Copper node,
- 4-Nitrophenol
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