3D N-heterocyclic covalent organic frameworks for urea photosynthesis from NH3 and CO2

Ning Li, Jiale Zhang, Xiangdong Xie, Kang Wang (), Dongdong Qi (), Jiang Liu, Ya-Qian Lan and Jianzhuang Jiang ()
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Ning Li: University of Science and Technology Beijing
Jiale Zhang: University of Science and Technology Beijing
Xiangdong Xie: South China Normal University
Kang Wang: University of Science and Technology Beijing
Dongdong Qi: University of Science and Technology Beijing
Jiang Liu: South China Normal University
Ya-Qian Lan: South China Normal University
Jianzhuang Jiang: University of Science and Technology Beijing

Nature Communications, 2025, vol. 16, issue 1, 1-10

Abstract: Abstract Artificial photosynthesis of urea from NH3 and CO2 seems to remain still essentially unexplored. Herein, three isomorphic three-dimensional covalent organic frameworks with twofold interpenetrated ffc topology are functionalized by benzene, pyrazine, and tetrazine active moieties, respectively. A series of experiment results disclose the gradually enhanced conductivity, light-harvesting capacity, photogenerated carrier separation efficiency, and co-adsorption capacity towards NH3 and CO2 in the order of benzene-, pyrazine-, and tetrazine-containing framework. This in turn endows tetrazine-containing framework with superior photocatalytic activity towards urea production from NH3 and CO2 with the yield of 523 μmol g−1 h−1, 40 and 4 times higher than that for benzene- and pyrazine-containing framework, respectively, indicating the heterocyclic N microenvironment-dependent catalytic performance for these three photocatalysts. This is further confirmed by in-situ spectroscopic characterization and density functional theory calculations. This work lays a way towards sustainable photosynthesis of urea.

Date: 2025
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DOI: 10.1038/s41467-025-56307-w

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