Details

Autor(en) / Beteiligte

• Xu, Hai-Qun
• Hu, Jiahua
• Wang, Dengke
• Li, Zhaohui
• Zhang, Qun
• Luo, Yi
• Yu, Shu-Hong
• Jiang, Hai-Long

Titel

Visible-Light Photoreduction of CO2 in a Metal–Organic Framework: Boosting Electron–Hole Separation via Electron Trap States

Ist Teil von

• Journal of the American Chemical Society, 2015-10, Vol.137 (42), p.13440-13443

Ort / Verlag

United States: American Chemical Society

Erscheinungsjahr

2015

Link zum Volltext

Quelle

Alma/SFX Local Collection

Beschreibungen/Notizen

• It is highly desirable to convert CO2 to valuable fuels or chemicals by means of solar energy, which requires CO2 enrichment around photo­catalysts from the atmosphere. Here we demonstrate that a porphyrin-involved metal–organic framework (MOF), PCN-222, can selectively capture and further photo­reduce CO2 with high efficiency under visible-light irradiation. Mechanistic information gleaned from ultrafast transient absorption spectroscopy (combined with time-resolved photoluminescence spectroscopy) has elucidated the relationship between the photo­catalytic activity and the electron–hole separation efficiency. The presence of a deep electron trap state in PCN-222 effectively inhibits the detrimental, radiative electron–hole recombination. As a direct result, PCN-222 significantly enhances photo­catalytic conversion of CO2 into formate anion compared to the corresponding porphyrin ligand itself. This work provides important insights into the design of MOF-based materials for CO2 capture and photo­reduction.