A 7 mL Teflon™ milling vessel equipped with one 12 mm stainless steel ball, was charged with (2,2,6,6tetramethylpiperidin-1-yl)oxyl (TEMPO, 5 mol%), N-methyl imidazole (NMI, 15 mol%), 2,2'-bipyridine (bpy) ligand (5 mol%), and [Cu(CN)4](OTf) (5 mol%). The closed Teflon™ vessel was mounted into the holding station of an IST636 mixer mill and milling was conducted at a frequency of 36 Hz for 1 minute. Subsequently, the milling vessel was opened, and 4-biphenyl methanol (IV) (0.5 mmol, 1 equiv.) was added to the vessel. The vessel was closed and mounted again into the mixer mill's holding station and milling was continued for 15 minutes in total. After each 5 minutes, the milling process was interrupted, and the vessel was opened for 2 minutes to allow for air exchange. After complete oxidation, the preformed ylide-created by milling the PPh3MeBr (0.9 mmol, 1.8 equiv.) and KO t Bu (0.8 mmol, 1.6 equiv.) for one minute in a separate vessel-was added as a yellow paste to the aldehyde-containing vessel. Subsequently, milling was continued for 1 minute.