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That was from the first episode Jigglypuff appeared in the first series, (The Song of Jigglypuff?). The scene was edited out when televised in the US, but it was supposedly uncut on VHS or DVD.
I remember I ripped this scene... ages ago. I doubt this is my clip but I don't know either way - I lost my own version and completely forgot about it. -__-
You DON'T want to know how hard it is to find an uncut version of this clip in an anime, all the pokemon series in all the different countries have their episodes shown in a different order and released on DVD in different orders too.
The episode IS the jigglypuff episode (one of the funniest, except for the Psyduck series)