Now him grabbing Holly in the first place was pure desperation, but when he has that change of heart I think he finally gave up on his delusions of having a 'family' – He knows he can only cause them pain at this point, so he just goes full Heisenberg on Skyler to both hurt and exonerate her. There's no coming back from any of that shit.

I don't think he'll make another attempt to make amends or even contact his family again. But I do think his final mission will have something to do with seeing to it that they get his meth money before he pops a ricin.