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Did the most damage... But I'm not sure he's villainous. Just competently dangerous. Happy to be corrected but I thought tmjr was trying to improve the world. He just got massively unlucky... Multiple times.
The effects of lead poisoning were already very well known, 8 people died of lead poisoning at DuPont during the development and Midgely himself suffered the effects of lead poisoning after "proving" his compound was safe in a public demonstration.
He absolutely knew there would have been widescale negative health effects if they continued to push the product on the market. He also knew about widely available alternative "anti-knocking" agents they could have used but they were unable to be patented and so there was no profit.
He is absolutely a case of someone who simply did not care about the consequences of his work beyond what profit could be extracted.
CFCs are a slightly different issue because no one could have reasonably anticipate their effects on the atmosphere and he was long dead before those effects were starting to be felt.
I don't believe he would have stopped developing them even if he did know however.
The universe got the last laugh however after he became entangled in self made contraption to help him after he developed polio, suffocating him.
Yeah, I'm pretty sure he invented freon use in refrigeration because he knew he fucked up with the lead in gasoline and wanted to do something good to outweight that.