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<p>The electrocatalytic oxidation of glycerol to produce high-value-added chemicals (<i>e.g.</i>, glycerate, GLA) constitutes a crucial process for harnessing the potential of glycerol. However, the high electrocatalytic activity is typically accompanied by catalyst deactivation by strong adsorption of the intermediates or products. Here, the Pt/RENC catalyst was prepared with small Pt nanoparticles supported on rare earth single-atom nitrogen-carbon (RENC, RE = La, Ce, Pr, Y) material. Aberration-corrected scanning transmission electron microscopy and X-ray absorption spectra confirm that the highly dispersed Ce sites are well maintained after the <i>in situ</i> formation of the Pt nanoparticles. The kinetic experiments, <i>in situ</i> IR and valence band characterizations, reveal that the synergy of a single atom of Ce-N<sub><i>x</i></sub> sites and Pt nanoparticles leads to the alleviation of the strong adsorption of GLA, and the enhancement of the H<sub>2</sub>O dissociation into active OH*, resulting in the fast conversion of glycerol. The rare earth single-atom sites also improve the anchoring of Pt nanoparticles. Remarkably, even in a high glycerol concentration of 0.6 M, the Pt/CeNC catalyst achieves a fast GLA production rate of 233 mmol h<sup>−1</sup> g<sub>Pt</sub><sup>−1</sup> and GLA yield of 51.7% with superior cycling stability, tripling the performance of the counterpart Pt/NC catalyst (75 mmol h<sup>−1</sup> g<sub>Pt</sub><sup>−1</sup> and 15.0%).</p>

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Synergy of rare earth single atoms and Pt nanoparticles for efficient electro-oxidation of glycerol into glycerate

  • 期刊论文

  • 发表日期：

    2025年4月8日

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  • Tao Chen,
  • Liang Lv,
  • Jing Yu,
  • Junfeng Du,
  • Zihan Ma,
  • Chaohui Guan,
  • Hang Wei,
  • Haibin Chu

摘要

The electrocatalytic oxidation of glycerol to produce high-value-added chemicals (e.g., glycerate, GLA) constitutes a crucial process for harnessing the potential of glycerol. However, the high electrocatalytic activity is typically accompanied by catalyst deactivation by strong adsorption of the intermediates or products. Here, the Pt/RENC catalyst was prepared with small Pt nanoparticles supported on rare earth single-atom nitrogen-carbon (RENC, RE = La, Ce, Pr, Y) material. Aberration-corrected scanning transmission electron microscopy and X-ray absorption spectra confirm that the highly dispersed Ce sites are well maintained after the in situ formation of the Pt nanoparticles. The kinetic experiments, in situ IR and valence band characterizations, reveal that the synergy of a single atom of Ce-Nx sites and Pt nanoparticles leads to the alleviation of the strong adsorption of GLA, and the enhancement of the H2O dissociation into active OH*, resulting in the fast conversion of glycerol. The rare earth single-atom sites also improve the anchoring of Pt nanoparticles. Remarkably, even in a high glycerol concentration of 0.6 M, the Pt/CeNC catalyst achieves a fast GLA production rate of 233 mmol h−1 gPt−1 and GLA yield of 51.7% with superior cycling stability, tripling the performance of the counterpart Pt/NC catalyst (75 mmol h−1 gPt−1 and 15.0%).