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An X-ray diffraction study and the solution chemistry is reported for the very stable ion pair [Ph3P=NH+2][TcO−4]. This compound crystallizes in the orthorhombic system, in space group P212121, with cell dimensions of a = 11.1454(6), b = 11.449(2), and c = 14.570(2)Å, and refining to R = 0.023 and RW = 0.031. Strong hydrogen bonds are formed between the iminium protons and the pertechnetate oxygens...