Atomically Precise Supported Au<sub>15</sub> Nanoclusters for Efficient and Selective Electrooxidation of Lignin-Derived Alcohols to Aromatic Ketones.
basic_science · Level V
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- Record sourced from PubMed, PMID 42456130.
- Also identified by DOI 10.1021/acs.nanolett.6c01582.
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Abstract
Selective electrooxidation of lignin-derived alcohols to value-added aromatic ketones enables sustainable biomass valorization, but remains limited by high overpotentials and competing C-C bond cleavage. Here, atomically precise Au<sub>15</sub> nanoclusters supported on carbon black (Au<sub>15</sub>/CB) were prepared through a ligand-stabilized rapid pyrolysis strategy. Au-S-C anchoring preserves the discrete electronic structure of Au<sub>15</sub> during immobilization. For 1-phenylethanol (1-PL) electrooxidation, Au<sub>15</sub>/CB delivers 10 mA cm<sup>-2</sup> at 0.96 V versus RHE, representing a 650 mV potential decrease relative to the oxygen evolution reaction. It also achieves 94% conversion of 1-PL with 99% selectivity toward acetophenone and excellent cycling stability, outperforming its single-atom (Au<sub>1</sub>/CB) and nanoparticle (Au NPs/CB) counterparts. Mechanistic studies show that an upshifted d-band center facilitates Au-OH<sub>ads</sub> formation and strengthens adsorption of key intermediates, thereby lowering the thermodynamic barrier while maintaining efficient product desorption. These findings highlight atomic precision as a strategy for selective biomass electro-upgrading.