Charge generation, charge transfer and charge utilization are three critical steps in photocatalysis, which jointly govern the overall efficiency for solar energy conversion. In our study, we develop a "three-in-one" strategy based on conjugated organic polymer (COP) coatings to synergistically intensify all three steps of charge generation, charge transfer and charge utilization for solar-powered regeneration of nicotinamide adenine dinucleotide (NADH). Under visible light illumination, the electrons generated from the triazine component in the COP coatings are transferred via imine bonds to the Rh cocatalyst in the COP coatings for subsequent utilization in NADH regeneration. The COP coatings can simultaneously intensify the charge generation and transfer, arising from the enhancement of light harvesting ability, lower interfacial electron transfer resistance and less electron-hole recombination. Moreover, the anchored Rh cocatalyst in the COP coatings can intensify the charge utilization as evidenced by the open circuit potential. The turnover frequency (TOF) of SiPP@COP-Rh toward NADH regeneration can reach 44.8 h<sup>-1</sup>, over 3.46-fold higher than that of bulk COP with free Rh cocatalyst. Our study may offer a generic strategy to elevate the catalytic efficiency through multi-component and multi-function integrative design in one single catalyst.

Three-in-one strategy <i>via</i> conjugated organic polymer coatings for solar-powered nadh regeneration

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Three-in-one strategy via conjugated organic polymer coatings for solar-powered nadh regeneration