Abstract: The terminal zirconium phosphinidene complex CpzZr (PR*)(PMe3)(R*= C&-2, 4, 6- t-Bu3) 2 has been synthesized in high yield, and its reactivity has been investigated. The compound CpzZrMe (PHR*) 1 is unstable with respect to the loss of methane; in the presence of PMe3 this reaction yielded 2. Reactions of 2 with benzophenone, benzaldehyde, or isophthalaldehyde produced phosphaalkenes PhCH= PR* 3, PhzC= ...