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I stumbled upon this sentence:

I accuse myself and others as having been irrational in the way we have been using statistics on a key notion of rationality.

Is there a difference in meaning/usage between "accuse X as" and "accuse X of"? Are they used in different contexts? Intuitively I prefer "accuse X of" every time.

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    I don't think there's a difference. I wouldn't use "accuse X as irrational" here either but "accuse X of being irrational". There may be a dialect where "as" is normal, though. It's really hard to make absolutist statements about usage when so many people use the language and so many are convinced that because they're native speakers, their usage is always correct, except for those obvious moments when even perfect knowledge of one's own idiolect fails and one misspeaks. That's a failing of many a politician, I've noticed, especially over the past 12 months.
    – user21497
    Nov 23 '12 at 15:28
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    There's certainly a difference in usage statistics. Google Books accused as:468K hits, accused of:11,400K hits. Using "as" in contexts where "of" would be valid conveys nothing to me apart from an indication of possible illiteracy. But it's fine in constructions like "stand accused as a {thief}", for example. Nov 23 '12 at 18:24
  • Just came across this for the first time: dmarge.com/2020/11/… Nov 28 '20 at 7:04
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You usually accuse [someone] of [some act of wrongdoing] (e.g. "I accuse him of bigamy").

Less commonly, you can accuse [someone] as [some type of wrongdoer], a form which often involves the passive voice, in conjunction with "stand" (e.g. "He stands accused as a bigamist").

Thus in OP's example, where having been irrational is a transgression/wrongdoing, the correct preposition is "of".

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