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For somebody that actually wants to be dead, nitrogen is the most painless method I am aware of. The key is breathe 100% nitrogen little or no recycled breath or atmosphere air, and have this continue for several minutes. There is no choking sensation or pain. You just get light-headed and pass out and eventually die of hypoxia.
Look at this video. This guy is training to be a fighter pilot. They put you in a high altitude chamber to create hypoxic effects so you know what to recognize when you're in the air. Fighter pilots breathe pure oxygen delivered through a series of regulators, gang load your regulator means manually select maximum flow rate on all regulators. So the point of this training is to recognize when you get hypoxic so you can crank up your oxygen.
Point is though, that guy isn't suffering. He's having a blast. He will keep holding up the wrong card and calling it four of spades all day. But that is what happens when the brain is starved of oxygen. If they reduce the oxygen level even farther in that chamber he would pass out, high enough and he would eventually die from it. Breathing 100% nitrogen at sea level does the exact same thing.
One assisted suicide group built a sort of death pod around this concept. I'm sure you can find it on Google. But the basic concept is it's an enclosure and when you push a button on the inside, a liquid nitrogen tank in the base starts delivering gaseous nitrogen to the pod in enough quantity to push away any CO2 you exhale. They put a ton of research into it, like it has safety interlocks and override switches and I think it can even play music.
For whatever it's worth, I hope you never have reason to make use of this information. I believe all life is precious.
But I also think that for somebody with a degenerative disease who's quality of life is going downhill who absolutely 100% is not going to get better, I think the option of choosing to die with dignity rather than suffer for a few more years in an expensive hospital in constant pain is something that should be available. I think that's a very personal decision and there's nobody on the fucking planet who has any right to make it for anyone other than themself.