Citation: Mingrun Li, Bin Han, Lei Gong, Yucheng Jin, Mingyue Wang, Xu Ding, Dongdong Qi, Jianzhuang Jiang. 1D COFs with phthalocyanine functional building blocks and imide linkage for superior electrocatalytic nitrate reduction[J]. Chinese Chemical Letters, ;2026, 37(2): 110590. doi: 10.1016/j.cclet.2024.110590 shu

1D COFs with phthalocyanine functional building blocks and imide linkage for superior electrocatalytic nitrate reduction

Mingrun Li ^a ,
Bin Han ^{a, *,} ,
Lei Gong ^b ,
Yucheng Jin ^a ,
Mingyue Wang ^a ,
Xu Ding ^a ,
Dongdong Qi ^a ,
Jianzhuang Jiang ^{a, *,}

a.
Beijing Advanced Innovation Center for Materials Genome Engineering, Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline Materials, Department of Chemistry and Chemical Engineering, School of Chemistry and Biological Engineering, University of Science and Technology Beijing, Beijing 100083, China
b.
National University of Singapore (Suzhou) Research Institute, Suzhou 215123, China

hanbin@ustb.edu.cn

jianzhuang@ustb.edu.cn

Received Date: 19 September 2024
Revised Date: 17 October 2024
Accepted Date: 29 October 2024
Available Online: 30 October 2024

Figures(6)

In comparison with their 2D and 3D counterparts, 1D covalent organic frameworks (COFs) have rarely been investigated due to the synthetic challenge arising from the strict necessary matching in the molecular symmetry between corresponding building blocks and linking units in addition to the unmanageable packing of 1D organic chains once formed. Herein, two novel imide-linked 1D COFs with phthalocyanine building blocks, namely NiPc-CZDM-COF and NiPc-CZDL-COF, were fabricated from the hydrothermal synthesis reaction of 2,3,9,10,16,17,23,24-octacarboxyphthalocyaninato nickel(Ⅱ) (NiPc(COOH)₈) with 9H-carbazole-3,6-diamine (CZDM) and 4,4′-(9H-carbazole-3,6-diyl)dianiline (CZDL), respectively. Two COFs have high crystallinity on the basis of powder X-ray diffraction analysis and high-resolution transmission electron microscopy. Due to their high ratio of exposed active centers on the edge sites of porous ribbons, both NiPc-CZDM-COF and NiPc-CZDL-COF electrodes display high utilization efficiency of NiPc electroactive sites of 8.0% and 7.5% according to the electrochemical measurement, resulting in their excellent capacity toward electrocatalytic nitrate reduction with the nitrate-to-NH₃ Faradaic efficiency of nearly 100%. In particular, NiPc-CZDM-COF electrode exhibits superior electrocatalytic performance with high NH₃ partial current density of −246 mA/cm², ammonia yield rate of 19.5 mg cm⁻² h⁻¹, and turnover frequency of 5.8 s⁻¹ at −1.2 V in an H-type cell associated with its higher conductivity. This work reveals the good potential of 1D porous crystalline materials in electrocatalysis.
- One-dimensional,
- Covalent organic framework,
- Phthalocyanine,
- Nitrate reduction,
- Electrocatalysis
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