Schlenk flask was charged with H2btdd (0.300 g, 1.13 mmol, 1.00 equiv.), N,Ndimethylformamidium trifluoromethanesulfonate (1.26 g, 5.63 mmol, 5.00 equiv.), and 130 mL of N,N-dimethylformamide (DMF). A solution of anhydrous manganese acetate (0.331 g, 1.92 mmol, 1.70 equiv.) in 20 mL of methanol was then added to the beige suspension. The flask was sealed, and the mixture was stirred at 125 °C for 7 days, during which a fine beige powder precipitated. This powder was collected by filtration over a fine porosity frit and subsequently suspended in ~15 mL of DMF and heated at 120 °C for 4 h. The supernatant was subsequently decanted and replaced with ~15 mL of fresh DMF five times. Additional solvent exchanges were then performed with ~15 mL of methanol at 60 °C four times, followed by ~10 mL of dichloromethane at room temperature twice. The dichloromethane-solvated material was subsequently activated under dynamic vacuum at 180 °C for 24 h to afford 0.417 g (85%) of product as a microcrystalline beige solid. Elemental analysis calcd for Mn5(CH3CO2)4(C12H4O2N6)3: C, 40.54%; H, 1.86%, N, 19.34%. Found: C, 35.94%; H, 1.48%; N, 16.89%.