Atomically Dispersed Pt–N3C1 Sites Enabling Efficient and Selective Electrocatalytic C–C Bond Cleavage in Lignin Models under Ambient Conditions

• DOI: 10.1021/jacs.1c02328
• Publication Date: 2021-06-17T19:24:30Z
• Authors: Tingting Cui; Lina Ma; Shibin Wang; Chenliang Ye; Xiao Liang; Zedong Zhang; Ge Meng; Lirong Zheng; Han-Shi Hu; Jiangwei Zhang; Haohong Duan; Dingsheng Wang; Yadong Li
• Keywords: Bond cleavage; Benzaldehyde; Noble metal

Selective cleavage of C–C linkages is the key and a challenge for lignin degradation to harvest value-added aromatic compounds. To this end, electrocatalytic oxidation presents promising technique by virtue mild reaction conditions strong sustainability. However, existing electrocatalysts (traditional bulk metal oxides) bond oxidative suffer from poor selectivity low product yields. We show first time that atomically dispersed Pt–N3C1 sites planted on nitrogen-doped carbon nanotubes (Pt1/N-CNTs), constructed via stepwise polymerization–carbonization–electrostatic adsorption strategy, are highly active selective toward Cα–Cβ in β-O-4 model compounds under ambient conditions. Pt1/N-CNTs exhibits 99% substrate conversion with 81% yield benzaldehyde, which exceptional unprecedented compared previously reported electrocatalysts. Moreover, using only 0.41 wt % Pt achieved much higher benzaldehyde than those state-of-the-art electrode (100 Pt) commercial Pt/C catalyst (20 Pt). Systematic experimental investigation together density functional theory (DFT) calculation suggests superior performance arises facilitating formation Cβ radical intermediate, further inducing radical/radical cross-coupling path break bond. This work opens up opportunities valorization green sustainable electrochemical route ultralow noble usage.