CO 2 ‐Folded Single‐Chain Nanoparticles as Recyclable, Improved Carboxylase Mimics

Emulating the function of natural carboxylases to convert CO 2 under atmospheric condition is a great challenge. Herein we report a class of CO 2 ‐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 CO 2 , which endows the SCNPs with extraordinary catalytic ability that can not only catalyze CO 2 ‐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.