Toluene oxidation with triple-module cooperativity in an atomically precise Cu4Pt2(C≡CCyOH)8 catalyst

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ID: 315283
2026
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Abstract
Abstract The dismantling and reassembly of C(sp3)-H bonds in hydrocarbons over both heterogeneous and homogeneous catalysts remain a fundamental challenge. Here we report the toluene oxidation using an atomically precise Cu4Pt2(C≡CCyOH)8 cluster (HC≡CCyOH = 1-ethynyl-1-cyclohexanol) as the electrocatalyst with an exclusive selectivity for benzaldehyde accompanied by >99% Faradaic efficiency. Results reveal the systematic cooperativity of three functional modules combined into one cluster catalyst for six temporally subsequent events: the hydroxyl ligand of this cluster can capture water and then release it to the Cu sites, and water is sequentially activated on the Cu sites to form OH radicals; Pt sites engage in the abstraction of a hydrogen atom from the methyl group of toluene; the OH radicals then flip over to the Pt sties and react with dehydro-toluene to produce benzaldehyde, which is finally disentangled from the active sites with the help of the ligand. Meanwhile, the cluster is also used to catalyze the hydrogen evolution reaction at the cathode and exhibits much higher activity for hydrogen production than a typical Pt/C catalyst. Our study presents a molecular approach for designing highly active and selective catalysts for efficient inert molecule-involved reactions.
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Authors Shisi Tang, Chenyang Shen, Qingxi Zhai, 田一淇, Mingchen Han, Dan Luo, Gongde Wu, Xiuwen Wang, Weiping Ding, Y C Zhu
Journal national science review
Year 2026
DOI
10.1093/nsr/nwag328
URL
https://doi.org/10.1093/nsr/nwag328
Keywords Keywords not found

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