Citation: Kun Zhang, Lei Wu, Kaixi Lan, Yanting Zhang, Wenxin Zhang, Huanhuan Li, Guoji Huang, Dongshuang Wu, Long Chen, Manni Li. N-3 of 1-methylimidazole: Enhancing proton conduction in COF under humidity conditions[J]. Chinese Chemical Letters, ;2026, 37(6): 111043. doi: 10.1016/j.cclet.2025.111043 shu

N-3 of 1-methylimidazole: Enhancing proton conduction in COF under humidity conditions

Kun Zhang ^{a, 1*,} ,
Lei Wu ^{a, 1} ,
Kaixi Lan ^{a, 1} ,
Yanting Zhang ^a ,
Wenxin Zhang ^a ,
Huanhuan Li ^a ,
Guoji Huang ^{b, *,} ,
Dongshuang Wu ^c ,
Long Chen ^a ,
Manni Li ^{a, *,}

a.
Automotive Engineering Research Institute, Jiangsu University. Zhenjiang 212013, China
b.
School of Resource & Environment, Nanchang University, Nanchang 330031, China
c.
School of Material Science and Engineering, Nanyang Technological University, Singapore 639798, Singapore

kunzhang@ujs.edu.cn

ghuang@ncu.edu.cn

lmn@ujs.edu.cn

Received Date: 21 January 2025
Revised Date: 19 February 2025
Accepted Date: 5 March 2025
Available Online: 14 March 2025

Figures(5)

The proton conduction mechanism of imidazole and its homologues within confined spaces has attracted much attention from researchers, which is highly beneficial for the development of novel proton exchange membranes. Traditionally, the hydrogen at the 1-position (H-1) on the nitrogen (N-1) of imidazole is seen as the exclusive source of mobile protons. However, we suggest that the 3-position nitrogen atom (N-3) can also generate mobile protons under hydrous conditions. This is because N-3 can form hydrogen bonds with water, which are particularly robust in confined spaces, thereby enhancing proton ionization from water and facilitating proton transfer. Based on this concept, 1-methylimidazole was introduced into a covalent organic framework (COF), resulting in a remarkable proton conductivity of 2.40 × 10^–3 S/cm at 70 ℃ and 100% relative humidity. This performance is on par with that of COFs doped with imidazole, demonstrating the key role of N-3···H₂O interactions within the framework in producing mobile protons and facilitating proton diffusion. Furthermore, this challenges the conventional viewpoint that H-1 of imidazole is the sole contributor to proton concentration, offering a new strategy for the preparation of high-performance proton conductors.
- Covalent-organic frameworks (COFs),
- 1-Methylimidazole,
- Imidazole,
- Proton conduction,
- H-bond interaction
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沈阳化工大学材料科学与工程学院沈阳 110142