Self-Assembly of Albumin and [FeFe]-Hydrogenase Mimics for Photocatalytic Hydrogen Evolution.

To imitate the protein microenvironment surrounding the Fe 2 S 2 active site, we established a convenient method to prepare self-assembled ovalbumin (OVA) nanogels that noncovalently incorporated hydrophobic FeFe-H 2 ase mimic (FeFe-1) in situ with an excellent loading efficiency up to 53.9%. The OVA@FeFe-1 composite nanogels (CG) were applied to photocatalytic hydrogen evolution in aqueous solution and exhibited improved catalytic efficiency with a turnover number amplified over 15 times relative to free FeFe-1 catalysts. The enhanced activity was attributed to the enrichment of the FeFe-1 catalyst and changes of protein secondary structures and microenvironment.