Using a Raman microprobe technique, we have measured the Raman spectra of singile crystaillites of Ti2Ba2Ca-lCu02fl+4-d (n1,2 and 3) with Tc varied by oxygen removal or addition. It is found in Ti2Ba2CuO6-d that the phonon modes associated with the vibrations of bridging 02 in Ba-0 planes (-"485 cnr') and 03 in 11-0 pianes (--600 cm ' ) increase i n frequency and become broader as the Ic increases from 0 to 70 K with oxygen removai, whiie the Ba and TIE vibration modes do not change appreciabily. The observations are attributed to the vallence change of TI., resuilting from a change in the charge transfer between H and (Cu-Ol), and to the distortion and/or disorder in 11-0 planes due to the oxygen removal.. In TI2Ba2CaCu2O8d and TlI2Ba2Ca2Cu3OlOd, the frequencies of 02 and 03 vibration modes increase with Tc raised by oxygen addition, while the Iow-frequency modes do not change. There is a ciear correlEation between Tc and phonon frequencies in fl-based superconductors. We suggest that a change in charge distribution in (Cu-01)-02-(fl-03) complexes is responsibEe for the phonon frequency shifts observed in 02 and 03 vibration modes.