Details

Autor(en) / Beteiligte

• Lu, Meng
• Li, Qiang
• Liu, Jiang
• Zhang, Feng-Ming
• Zhang, Lei
• Wang, Jin-Lan
• Kang, Zhen-Hui
• Lan, Ya-Qian

Titel

Installing earth-abundant metal active centers to covalent organic frameworks for efficient heterogeneous photocatalytic CO2 reduction

Ist Teil von

• Applied catalysis. B, Environmental, 2019-10, Vol.254, p.624-633

Ort / Verlag

Amsterdam: Elsevier B.V

Erscheinungsjahr

2019

Quelle

Alma/SFX Local Collection

Beschreibungen/Notizen

• A novel heterogeneous catalytic system based on earth abundant metal-modified covalent organic frameworks was designed and applied in photocatalytic CO2 reduction. Noted that the DQTP COF-Co species presented the highest CO production rate (1.02 × 103 μmol h−1 g−1) and the reductive product selectivity (CO/HCOOH) can be adjusted by loading different metal active centers. [Display omitted] •A metal-modified COFs system was designed for heterogeneous CO2 photoreduction.•The catalytic activity/selectivity can be tuned by different metal-based COFs.•DQTP COF-Co/Zn exhibited superior CO/formic acid production performance.•A mechanism for photocatalytic CO2 reduction over metal-modified COFs was proposed.•A model COF system was afforded for effective bonding open metal active centers. Photocatalytic conversion of CO2 into energy carriers has been recognized as a highly promising strategy for achieving the virtuous carbon cycle in nature. The realization of this process depends on an efficient catalyst to reduce the reaction barrier. Herein, we report a series of transition metal ion modified crystalline covalent organic frameworks (COFs) for the heterogeneous photocatalytic reduction of CO2. By coordinating different kinds of open metal active species into COFs, the resultant DQTP (2,6-diaminoanthraquinone - 2,4,6-triformylphloroglucinol) COF-M (M = Co/Ni/Zn) exerts a strong influence on the activity and selectivity of products (CO or HCOOH). Significantly, DQTP COF-Co exhibits a high CO production rate of 1.02 × 103 μmol h−1 g−1, while DQTP COF-Zn has a high selectivity (90% over CO) for formic acid generation (152.5 μmol h−1 g−1). This work highlights the great potential of using stable COFs as platforms to anchor earth-abundant metal active sites for heterogeneous CO2 reduction.