Abstract
Enzymatic catalytic processes possess great potential in chemical manufacturing, including pharmaceuticals, fuel production and food processing. However, the engineering of enzymes is severely hampered due to their low operational stability and difficulty of reuse. Here, we develop a series of stable metal-organic frameworks with rationally designed ultra-large mesoporous cages as single-molecule traps (SMTs) for enzyme encapsulation. With a high concentration of mesoporous cages as SMTs, PCN-333(Al) encapsulates three enzymes with record-high loadings and recyclability. Immobilized enzymes that most likely undergo single-enzyme encapsulation (SEE) show smaller Km than free enzymes while maintaining comparable catalytic efficiency. Under harsh conditions, the enzyme in SEE exhibits better performance than free enzyme, showing the effectiveness of SEE in preventing enzyme aggregation or denaturation. With extraordinarily large pore size and excellent chemical stability, PCN-333 may be of interest not only for enzyme encapsulation, but also for entrapment of other nanoscaled functional moieties.
Highlights
Enzymatic catalytic processes possess great potential in chemical manufacturing, including pharmaceuticals, fuel production and food processing
On the basis of structural rationalization, we report facile syntheses of a series of highly stable single-molecule traps (SMTs)-containing Metal-organic frameworks (MOFs) based on trivalent metal species, namely PCN-332(M) (M 1⁄4 Al(III), Fe(III), Sc(III), V(III), In(III)) and PCN-333(M) (M 1⁄4 Al(III), Fe(III), Sc(III))
From a pure size-match point of view, horseradish peroxidase (HRP) and cytochrome c (Cyt c) will most likely undergo single-enzyme encapsulation (SEE), whereas MP-11 will go through multiple-enzyme encapsulation (MEE) due to size mismatch
Summary
Enzymatic catalytic processes possess great potential in chemical manufacturing, including pharmaceuticals, fuel production and food processing. We develop a series of stable metal-organic frameworks with rationally designed ultra-large mesoporous cages as single-molecule traps (SMTs) for enzyme encapsulation. Mesoporous silica nanoparticles, which have a large pore size, high porosity and a very ordered structure, have been demonstrated as promising enzyme supports[5]. Due to their one-dimensional (1D) channel structure, insufficient interactions between the inner channel surface of mesoporous silica and enzymes result in significant leaching during multiple cycles of use. C3h high loading amounts among all reported solid supports These immobilized enzymes either maintain or surpass their catalytic activities over the free enzymes, and exhibit smaller Km and better catalytic performance in organic solvents. These immobilized enzymes show almost no leaching during catalysis and recycling, and maintain high catalytic activity
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