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I'm not a rubber chemist, but I would think that aging rubber would make the internal friction (hysteresis) higher and that is the largest contributor to rolling resistance. I would tend to think this would be a small change and certainly not as dramatic as you have posted. So I tend to think that the answer lies elsewhere.
One possibility is that given the wide range of values of rolling resistance within a given size, it is much more likely that the difference is caused by the inherent difference between the current set and the previous set.
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