Artificial photosynthesis platform of 2D/2D MXene/crystalline covalent organic frameworks heterostructure for efficient photoenzymatic CO2 reduction

• Published in: Applied catalysis. B, Environmental Environmental, 2024-07, Vol.348, p.123827, Article 123827
• Main Authors: Qu, Jiafu, Yang, Tingyu, Zhang, Pengye, Yang, Fengyi, Cai, Yahui, Yang, Xiaogang, Li, Chang Ming, Hu, Jundie
• Format: Article
• Language: English
• Subjects: Artificial photosynthesis; CO2 reduction; Covalent organic frameworks; NADH regeneration; Photoenzymatic catalysis
• ISSN: 0926-3373; 1873-3883
• DOI: 10.1016/j.apcatb.2024.123827

Photoenzymatic catalysis is an efficient strategy for selectively converting CO2 into valuable chemicals. However, the sluggish reaction kinetics, resulting from low visible light utilization and rapid recombination of photogenerated carriers, severely inhibit the yields of target products. Herein, we present a novel artificial photosynthesis platform of 2D/2D MXene/crystalline COF-367 heterostructure for efficient conversion of CO2 into HCOOH. This platform is extremely sensitive to solar light (λ ≤ 750 nm), with rapid charge separation and transfer due to the well-designed abundant ultrathin 2D/2D hetero-interfaces. Remarkably, Ti3C2/COF-367 achieves an impressive yield of 83.38% for coenzyme NADH regeneration with absence of electron mediator. Furthermore, it demonstrates a cascade ultra-high production rate of HCOOH at 1.88 mmol g−1 h−1 with almost 100 % selectivity. This work represents the first example of MXene to promote charge transfer in COFs-based photoenzymatic synergistic catalytic system, and provides insights into the development of organic/inorganic hybrids for CO2 photoreduction. [Display omitted] •First example of MXene to promote charge transfer in COFs-based photoenzymatic catalytic system.•Ultrathin highly crystalline imine-linked COF-367 nanosheets were synthesized.•Abundant ultrathin 2D/2D hetero-interfaces for rapid charge separation/transfer.•Impressive NADH regeneration yield of 83.38% without electron mediator.•Ultra-high HCOOH production rate of 1.88 mmol g−1 h−1 with high selectivity.