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K-mediated peripheral electronic tuning of low-valence Au single atoms for efficient acetylene hydrochlorination
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张
H
DOI：10.1039/D6GC01092J.png)
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Abstract
En 中文
Gold single-atom catalysts hold great promise for acetylene hydrochlorination; yet their practical application is hindered by the instability and reduction tendency of high-valence Au species. Herein; we report a K-mediated peripheral electron regulation strategy for the construction of stable low-valence Au single-atom catalysts on nitrogen-doped carbon supports (Au/K-NC-SA). During a 400-hour stability test; the catalyst achieved a reaction rate of 812.1 kgVCM kgAu−1 h−1 and a deactivation rate of (7.6 ± 0.2) × 10−3% h−1. As an electron donor; K reduces the average oxidation state of Au; increases the electron density of Au 5d orbitals and upshifts the d-band center. This further strengthens the adsorption of acetylene and hydrogen chloride; stabilizes the key transition state; and reduces the energy barrier of the rate-determining step by 0.28 eV. Beyond providing a highly active and stable catalyst; this work deciphers the synergistic mechanism of electronic and field effects in the “K-mediated peripheral effect”; offering a general design principle for stabilizing single-atom catalysts with tailored electronic states; providing a feasible technical scheme for the green transformation of the coal-based polyvinyl chloride industry and aligning with the core principles of green chemistry.
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