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The following sentence has been painted on the wall in an education building of a major university

Harness your enthusiasm of learning.

Is this correct, or should it be

Harness your enthusiasm for learning."

or are both acceptable?

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  • enthusiasm for something. – Lambie Jul 12 '19 at 14:18
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Perhaps it might be different in the region where that university is located, or at the time that slogan was originally painted, but in the variety of English I'm familiar with (USA-type), that sentence does not sound quite idiomatic.

The typical preposition used with the object of enthusiasm is "for":

The dogs had a lot of enthusiasm for the treats.

He showed no enthusiasm for ballet.

His enthusiasm for music has stayed strong throughout his 23 years in radio. (Example used by MacMillan dictionary)

or as you propose,

Harness your enthusiasm for learning.

The preposition "of" (regarding enthusiasm) is usually reserved for the person or location where the enthusiasm resides (the ones who are enthusiastic):

The enthusiasm of the children was obvious.

I couldn't be depressed when confronted with the enthusiasm of the trainees.

It was inspiring to witness the enthusiasm of the Clean Campus Club for their task.

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  • I do not disagree with your answer overall. Indeed, I think it is an excellent answer, but I doubt that a place can have enthusiasm. Something like "New York has enthusiasm for the Yankees" refers to the people of New York and is figurative speech that substitutes the name of a place, e.g. Club, for people associated with that place. Minor point admittedly. – Jeff Morrow Jul 12 '19 at 14:27
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Both "enthusiasm of" and "enthusiasm for" are idiomatic expressions, but they mean different things.

The enthusiasm of a small child is infectious

relates to who is experiencing the emotion of enthusiasm.

He lost his enthusiasm for politics

relates to what elicits the emotion of enthusiasm.

Thus, the meaning probably intended by the painting you mention is not being expressed idiomatically (at least not in US English).

As a side note, this example demonstrates the danger of using ngram to determine what is idiomatic. Two usages may show as being common, but they have may distinct meanings and cannot idiomatically be substituted for each other.

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