Authors
Mengxue Kang, Yan Chu, Zhichun Xu, Jiao Feng, Ganlu Li, Kequan Chen, Hui Li
Published in
Advanced science (Weinheim, Baden-Wurttemberg, Germany). Pages e78027. Sep 27, 2026. Epub Sep 27, 2026.
Abstract
Integrated photo-enzymatic catalysis combines the merits of both photocatalytic and enzymatic systems; however, the spatial separation of photocatalysts and enzymes in conventional one-pot setups often limits overall efficiency due to sluggish electron transfer. To address this, we constructed a light-driven artificial metalloenzyme (Rh-L6-FDH) featuring dual catalytic centers by covalently conjugating formate dehydrogenase (FDH) with a tailored rhodium complex (Rh-L6), thereby facilitating synergistic NADH regeneration and CO2 conversion. Screening nine synthesized Rh complexes with structurally diverse ligands revealed that Rh-L6 exhibited the highest efficiency for light-driven NADH regeneration. Consequently, the resulting Rh-L6-FDH conjugate yielded formate with a 2.31-fold increase compared to the physical mixture of free FDH and Rh-L6. The enhancement is mechanistically linked to the combined effects of a narrowed bandgap, diminished activation energy, and the proximity between catalytic centers, which synergistically promote charge separation and CO2 activation. To overcome the inherent instability of the conjugate, Rh-L6-FDH was immobilized within a ZIF-67 framework. This strategy markedly improved catalytic robustness, boosting formate conversion to 98.4%-a 16.68-fold improvement over the free component system. This work demonstrates the potential of integrating molecular metal complexes with enzymes into a unified architecture, offering a promising pathway for sustainable cofactor regeneration and efficient carbon sequestration.
PMID:
42801539
Bibliographic data and abstract were imported from PubMed on 28 Sep 2026.
Read full publication at:
Please sign in
to see all details.
Advertisement
Stats
- Recommendations n/a n/a positive of 0 vote(s)
- Views 27
- Comments 0