Dimensionally Extended Homochiral Metal-Organic Frameworks for Catalysis and Enantioselective Sensing

• • Dimensional evolution from 1D/2D to 3D HMOFs achieved by tuning auxiliary ligand connectivity, yielding a novel 4-(3,3,3,6)-connected topology with heart-shaped channels, enabling dual functionality. • • P/M-HMOF-5 exhibit acid-base bifunctional heterogeneous catalysis for 2,3-dihydroquinazolinone synthesis with excellent yields of 90%–98%, demonstrating high efficiency and potential for industrial fine chemical production. • • M-HMOF-5 shows highest enantioselective fluorescent sensing for phenylalanine with KBH(D-Phe)/KBH(L-Phe) = 5.85, and for D-Phe recognition, KBH(M)/KBH(P) = 7.17, underscoring superior chiral discrimination for analytical applications. • • The integration of catalytic and sensing functions within a single chiral platform, derived from identical chiral building blocks, offers a rational strategy for designing multifunctional materials, reducing processing steps and material costs.