Controlling the Spatiotemporal Self-Organization of Stimuli-Responsive Nanocrystals under Out-of-Equilibrium Conditions.

Self-organization under out-of-equilibrium conditions is ubiquitous in natural systems for the generation of hierarchical solid-state patterns of complex structures with intricate properties. Efforts in applying this strategy to synthetic materials that mimic biological function have resulted in remarkable demonstrations of programmable self-healing and adaptive materials. However, the extension of these efforts to multifunctional stimuli-responsive solid-state materials across defined spatial distributions remains an unrealized technological opportunity.

Metallated Isoindigo-Porphyrin Covalent Organic Framework Photocatalyst with a Narrow Band Gap for Efficient CO Conversion.

Photocatalytic CO reduction into formate (HCOO) has been widely studied with semiconductor and molecule-based systems, but it is rarely investigated with covalent organic frameworks (COFs). Herein, we report a novel donor-acceptor COF named composed of isoindigo and metallated porphyrin subunits that exhibits high catalytic efficiency (∼50 μmol formate g h) at low-power visible-light irradiation and in the absence of rare metal cocatalysts. Density functional theory calculations and experimental diffuse-reflectance measurements are used to explain the origin of catalytic efficiency and the particularly low band gap (0.