Abstract
Continuous industrialization has raised daunting environmental concerns, and there is an urgent need to develop a sustainable strategy to tackle the contamination issues. Here, we report a supramolecular photoenzyme ensemble enabling the harvest of solar energy to remove contaminations in water. The well-sourced oxidoreductase, laccase, is confined into a photoactive hydrogen-bonded organic framework (PHOF) through an in situ encapsulation method. The direct electron migration between the oxidation center in a PHOF and the reduction center in laccase facilitates synergistic photoenzyme-coupled catalysis, showing two orders of magnitude higher activity than free laccase for pollutant degradation under visible light, without the need for sacrificial agents or costly co-mediators. Such high decontamination efficiency also surpasses the reported catalysts. The structure and decontamination function of this supramolecular photoenzyme ensemble remain highly stable in complex environment matrices, presenting desirable reusability and almost 100% conversion efficiency of pollutants for real sewage samples. Our conceptual photoenzyme hybrid catalyst offers important insights into green and sustainable water decontamination.