Design of high-efficiency carbonic anhydrase mimics with well-defined Zn sites based on salphen organic framework

Abstract

For a variety of CO2-related catalytic applications, developing reliable and efficient biocatalysts with carbonic anhydrase (CA)-like activities presents an appealing application potential. However, very limited progress has been made in regulating the activity of biocatalysts that can mimic the natural CA. Here, inspired by the Zn-coordination structure of CA active centers, we report a new and efficient CA-mimetic organic framework with Zn-N2O2 single-atom active sites to promote CO2-related hydration reactions. Because of the increased atomic utilization level compared to Zn coordinated salphen organic framework, the CA-like biocatalyst exhibits ultrafast reaction kinetics in p-NPA hydrolysis (V0 = 317.82nM s−1, Vmax = 1.28 µM s−1, turnover number: 3.91 × 10-3 s−1), which surpasses the majority of CA-mimetic biocatalysts that have been reported to date. Our research indicates that the construction of well-defined Zn centers and the improvement of atomic utilization efficiency can enhance the activity of CA-like biocatalysts and outline a new approach to regulating the catalytic activity of CA-mimicking biocatalysts for a wide range of CO2-related processes.