4.8 Article

Reversible Light-Controlled CO Adsorption via Tuning π-Complexation of Cu+ Sites in Azobenzene-Decorated Metal-Organic Frameworks

Journal

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 61, Issue 46, Pages -

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202212732

Keywords

CO Adsorption; Cu+ Sites; Light-Responsive Property; Smart Adsorbents; pi-Complexation Interaction

Funding

  1. National Science Fund for Distinguished Young Scholars [22125804]
  2. National Natural Science Foundation of China [22078155, 22008112]
  3. China Postdoctoral Science Foundation [2019M661813]
  4. Project of Priority Academic Program Development of Jiangsu Higher Education Institutions
  5. High Performance Computing Center of Nanjing Tech University

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This study reports a smart pi-complexation adsorbent that can adjust the pi-complexation of active sites via light irradiation, thereby regulating the performance of the adsorbent. The results show that the CO uptake of the adsorbent can be significantly changed by altering the light irradiation, providing a clue for designing target-specific smart materials.
Light-responsive adsorbents capture significant attention due to their tailorable performance upon light irradiation. The modulation of such adsorbents is mainly based on weak (physical) interactions caused by steric hindrance while tuning strong interaction with target adsorbates is scarce. Here we report smart pi-complexation adsorbents, which can adjust the pi-complexation of active sites via light irradiation. A typical metal-organic framework, MIL-101-NH2, was decorated with azobenzene motifs, and Cu+ as pi-complexation active sites were introduced subsequently. The reversible light-induced isomerization of azobenzene regulates the surface electrostatic potentials around Cu+ from -0.038 to 0.008 eV, causing shielding and exposure effects. The alteration of CO uptake is achieved up to 54 % via changing light, while that on MIL-101-NH2 is negligible. This study provides a clue for designing target-specific smart materials to meet the practical stimuli-responsive adsorption demands.

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