CO2-Folded Single-Chain Nanoparticles as Recyclable, Improved Carboxylase Mimics

摘要

Emulating the function of natural carboxylases to convert CO(2)under atmospheric condition is a great challenge. Herein we report a class of CO2-folded single-chain nanoparticles (SCNPs) that can function as recyclable, function-intensified carboxylase mimics. Lewis pair polymers containing bulky Lewis acidic and basic groups as the precursor, can bind CO(2)to drive an intramolecular folding into SCNPs, in which CO(2)as the folded nodes can form gas-bridged bonds. Such bridging linkages highly activate CO2, which endows the SCNPs with extraordinary catalytic ability that can not only catalyze CO2-insertion of C(sp(3))-H for imitating the natural enzyme's function, it can also act on non-natural carboxylation pathways for C(sp(2)and sp)-H substrates. The nanocatalysts are of highly catalytic efficiency and recyclability, and can work at room temperature and near ambient CO(2)condition, inspiring a new approach to sustainable C(1)utilization.