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I've heard nitrogen gas is perhaps the most humane method (though I oppose capital punishment). The feeling of asphyxiation comes from rising CO2 in the brainstem. If he can continue expelling the CO2 you won't feel anything except as you go hypoxic you'll become more dazed and confused until you simply pass out.
Then again I've always wondered why we don't just put these people under anesthesia and then overdose on morphine.
That one's in part because cruelty is by design I imagine, but also because the people giving those injections aren't medical professionals and can't legally obtain those substances. Guess that also explains how they can fuck up finding veins this bad. From what I've read and heard (In Last Week Tonight among others, I believe) they basically just use toxic crap that chemically burns the inmate from the inside and makes them asphyxiate while conscious. And of course they turn out to be undeserving of an execution around 5% of the time.
Wait, seriously? They aren't even medical professionals administering the substances...?
Guess that would kind of go against the Hippocratic Oath.