Enzyme-photo-coupled systems (EPCSs) offer a green strategy for producing high-value chemicals, but significant gaps remain in comparison to natural photosynthetic systems. Herein, we report an all-in-one EPCS (AiO-EPCS) by integrating photocatalytic (photocatalyst, P; electron mediator, M; electron donor, D) and biocatalytic (enzyme and cofactor) units in a hydrogen-bonded organic framework (HOF) for efficient NAD(P)H regeneration and light-driven enzymatic transformations, functioning like a chloroplast. The photocatalytic system assembled by incorporating P and M onto poly(allylamine hydrochloride) (PAH), PAHPM, exhibits an 11-fold enhanced photocatalytic NAD(P)H regeneration yield over the free mixture. Subsequently, two different AiO-EPCSs are fabricated by trapping two biocatalytic systems into HOF with the assistance of PAHPM. A double-layer architecture forms within the framework, partially separating the photo- and bio-catalytic modules while keeping all catalytic components in proximity. Moreover, adsorption of D onto HOF enables the system to be recycled by a single D addition, aligning AiO-EPCSs with natural photosynthesis in economic sustainability.
Liu et al. (Wed,) studied this question.