Issue 28, 2025

Dual-reaction-centre enabled concurrent N–C–N coupling for effective urea electrosynthesis

Abstract

Electrocatalytic C–N coupling offers a promising approach to producing urea economically and sustainably. However, the process is often hindered by complex reaction mechanisms and a lack of spatial functional differentiation between CO2 reduction and C–N coupling in catalysts. To address this issue, we propose designing dual-reaction-centre catalysts (DRCCs) with two spatially independent active sites, each dedicated to a critical reaction step. Through high-throughput methods and theoretical simulations, fifteen 2D metal–organic frameworks PcTM1–O8–TM2 complexes are identified, where TM1 = Ti, V, Cr, Mo, Tc and TM2 = Mn, Cr, Fe. These frameworks enable the synchronous activation of NO and CO2 on separate active centres, facilitating a concurrent N–C–N coupling mechanism. The CO produced by CO2 reduction at the TM2 site preferentially inserts into *NO–NO at the TM1 site, forming a unique *NOCONO precursor. The low onset potentials, reasonable kinetic barriers for N–C–N coupling, and high stability and selectivity of these DRCCs demonstrate outstanding catalytic performance comparable to the benchmark PdCu alloy.

Graphical abstract: Dual-reaction-centre enabled concurrent N–C–N coupling for effective urea electrosynthesis

Supplementary files

Article information

Article type
Paper
Submitted
17 Mar 2025
Accepted
10 Jun 2025
First published
12 Jun 2025

J. Mater. Chem. A, 2025,13, 22685-22694

Dual-reaction-centre enabled concurrent N–C–N coupling for effective urea electrosynthesis

J. Liu, S. C. Smith, X. Tan, Y. Gu and L. Kou, J. Mater. Chem. A, 2025, 13, 22685 DOI: 10.1039/D5TA02152A

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