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Strengthened d-π Interaction in Bimetallic Cluster for Boosted Urea Electrosynthesis from Nitrate and CO2 in Simulated Industrial Waste
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DOI：10.1039/D6GC02382G.png)
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Abstract
En 中文
Electrocatalytic conversion of NO3- and CO2 offers a viable strategy for waste resource utilization. However; current studies largely focuses on high-concentration systems; while efficient electrocatalytic synthesis under realistic low-concentration polluted conditions remains in its infancy. Herein; we report a bimetallic cluster CuI4FeII (CuI4FeII(PPh3)4L6; L = tetrazole) via strategic FeII-for-CuII substitution. The experiment shows that under the conditions of -0.64 V vs. RHE; 100% CO2 and 50 mM NO3-; the Faradaic efficiency (FE) of urea using this catalyst reaches 62%; which is twice that of CuI4CuII and is the best among the clusters. Under simulated real-world low-concentration conditions (20% CO2; 600 ppm NO3-); the CuI4FeII maintains a FE of 41% and exhibits robust catalytic performance across a wide range of CO2 and NO3- concentrations. Mechanistic studies reveal that the introduction of the Fe site induces significant electronic restructuring; which not only enhances NO3- adsorption and reduces its protonation energy barrier but also strengthens the d-π interactions between metal orbitals and key intermediates. This effect effectively lowers the overall reaction energy barriers and facilitates CO2 insertion and subsequent C–N coupling; thereby rationalizing the observed high catalytic activity. This work demonstrates heterometallic synergy for efficient multi-step electrocatalysis under practical conditions.
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