The first piece, already grilled, probably can't be tenderized unless you cut it into stew meat and make stew, gumbo, a gulasz, or maybe a chile or a pot pie.
To tenderize uncooked roast, I marinate in a mix of oil, vinegar, salt, pepper, garlic powder, maybe Italian seasonings or oregano, sage, basil, etc. I marinate my roast for approximately .1/2 to 1 hour, then put it on the pit. I cook it rare to medium rare and serve immediately if at all possible. I prefer chuck roast from the local butcher shop, not rubber faux roast from Wally World.
I found marinating over 1 hour makes it fall apart and it becomes more like a crock potted roast - not good for the grill.
If you take the cooked roast, throw it in a crock pot or slow cooker with taters, carrots, onions, tomatoes,
lots of butter, seasonings, etc, and cook it for about 4-6 hours (depending on size, add water if needed during cooking) it should fall apart with a fork, no knife needed, should be tender.
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