Authors
Nan-Nan Zhang, Ling-He Kong, Zhi-Hao Zhao, Xiu Qiao, Tian-Shu Song, Yan Sun, Ya Wang, Lu-Hua Shao, Hong Dong, Feng-Ming Zhang
Published in
Advanced materials (Deerfield Beach, Fla.). Pages e75407. Oct 16, 2026. Epub Oct 16, 2026.
Abstract
Photocatalytic urea synthesis directly from atmospheric CO2 and N2 offers a sustainable route to bypass the energy-intensive Bosch-Meiser process, yet simultaneously achieving CO2 capture and reduction, N2 activation, and C─N coupling within a single system remains challenging. Herein, we report a two-step tandem platform combining ionic-liquid-modified metal-organic framework (IL@PCN-250-Fe2Co) with a trinuclear copper-based covalent organic framework (HTP-Cu3-imi-COF) for urea photosynthesis from air. The IL@MOF captures atmospheric CO2 and photoreduces it to CO, while HTP-Cu3-imi-COF couples the generated CO with ambient N2 into urea. This synergistic tandem configuration delivers a urea production rate of 259.87 µg·gcat -1·h-1 under air, marking the first demonstration of photocatalytic urea synthesis from atmospheric CO2 and N2. In situ spectroscopic measurements and DFT calculations reveal that the imidazole-functionalized HTP segments act as hole-rich oxidation domains, promoting water oxidation to generate *OH species that oxidize locally enriched N2 to *NO intermediates. Simultaneously, the Cu3 clusters serve as electron-rich centers for CO adsorption and activation, forming *CO that couples with *NO via the critical *OCNO intermediate toward urea formation. This work not only showcases the first photocatalytic urea synthesis from air but also establishes a modular paradigm for cascade catalysts that integrate capture and conversion toward sustainable chemical transformations.
PMID:
42885386
Bibliographic data and abstract were imported from PubMed on 16 Oct 2026.
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