Anisotropic Defect-Induced Orbital Reordering Enables Coherent Charge Redistribution and Selective Photocatalytic CO2 Reduction in Metal-Organic Frameworks.
Photocatalytic CO2 reduction in metal-organic frameworks (MOFs) is often limited by inefficient charge separation and poorly defined active sites, while the role of crystallographic defect heterogeneity remains unclear. Taking MIL-125-NH2 as a prototypical system, we demonstrate that inequivalent oxygen vacancies dicta...