Abstract
Revealing the mechanism of photocatalytic organic transformation in aqueous solutions is crucial for photocatalytic processes, yet precisely regulating complex interfacial electron transfer and the microenvironment of reaction molecules remains challenging. Inspired by cellular structures and natural metalloproteins, we construct a ZIF-67@CoS/CdS nanoreactor mimicking organelle architecture. This system enables directional charge transport and hydrogen-bond microenvironment regulation, allowing efficient co-production of H2 and pyruvic acid under light irradiation. Characterizations and calculations reveal that the interfacial electric field accelerates charge migration, while the catalyst reduces the energy barriers for water dissociation and hydrogen formation by modulating hydrogen bonds. The optimized catalyst delivers a molar-level H2 activity of 1457.1 mmol m-2 (5 h, 1,000 cm2) under sunlight, with a pyruvic acid selectivity of 91.2%. In this work, we propose a design strategy for an organelle-mimetic nanoreactor for scalable sunlight-driven H2 production and selective pyruvic acid synthesis.