<p>Traditionally, adsorption is believed to take place only in the ground state, but here we report an excitation-driven adsorption mode. Composites of metallophthalocyanines and carbonaceous substrates are prepared, among which the potassium-phthalocyanine (KPc)/reduced graphene oxide (RG) composite shows the most typical behavior. Femtosecond transient absorption spectroscopy and first-principles simulations reveal that under ultraviolet (UV) irradiation, the excited electrons in the composite transfer efficiently from KPc to RG, leaving long-lived excited holes on KPc that enable selective adsorption of CO molecules. In the dark, the composite shows negligible CO adsorption (0.06 mmol g⁻<sup>1</sup>), whereas its CO uptake increases to 1.20 mmol g⁻<sup>1</sup> upon UV light, with a UV-modulated adsorption capacity ratio of up to 95%. This adsorption mode is also applicable to other metallophthalocyanine/carbonaceous composites. This work presents a potential strategy for photoexcitation utilization and the development of energy-efficient chemical separation technologies.</p>

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Adsorption based on excitation

  • Shi-Chao Qi,
  • Yan-Yan Han,
  • Yong-Lan Liu,
  • Yun-Jie Zhao,
  • Qi-Qi Huang,
  • Xiao-Qin Liu,
  • Lin-Bing Sun

摘要

Traditionally, adsorption is believed to take place only in the ground state, but here we report an excitation-driven adsorption mode. Composites of metallophthalocyanines and carbonaceous substrates are prepared, among which the potassium-phthalocyanine (KPc)/reduced graphene oxide (RG) composite shows the most typical behavior. Femtosecond transient absorption spectroscopy and first-principles simulations reveal that under ultraviolet (UV) irradiation, the excited electrons in the composite transfer efficiently from KPc to RG, leaving long-lived excited holes on KPc that enable selective adsorption of CO molecules. In the dark, the composite shows negligible CO adsorption (0.06 mmol g⁻1), whereas its CO uptake increases to 1.20 mmol g⁻1 upon UV light, with a UV-modulated adsorption capacity ratio of up to 95%. This adsorption mode is also applicable to other metallophthalocyanine/carbonaceous composites. This work presents a potential strategy for photoexcitation utilization and the development of energy-efficient chemical separation technologies.