No, ascension requires more than just knowledge
From what we are told, the repository of knowledge inserts knowledge into your brain, but does not otherwise alter your physical being. This is why the Asgard are able to reverse O'Neill's condition on the two occasions he was subjected to it; they simply removed the knowledge from his mind.
It basically downloads the entire library of Ancient knowledge into a person's mind. That massive amount of data then slowly unspools into your brain, eventually taking over your consciousness completely.
–Samantha Carter in Stargate SG-1, "Lost City, Part 1"
But does this help with ascension? There are two ways for a human to ascend: spiritual ascension and physical ascension.
This is the method that Daniel Jackson used to ascend. However, the path is not particularly straightforward, as he found out with Oma Desala.
Oma: When the mind is enlightened, the spirit is freed and the body matters not.
Daniel: You're talking about ascension, right? Rising to a different plane of existence. Are you saying that I could do that? Become like you?
Oma: You must complete the journey you began at Kheb. Only then will you be able to find your way to the Great Path.
Daniel: What do I do?
Oma: Release your burden.
Daniel: Okay, well, consider it released. What's Step Two?
Oma: A tall man cannot hide in the short grass.
Daniel: You know, I really, I don't have time for one of these kind of conversations.
–Stargate SG-1, "Meridian"
The repository of knowledge doesn't give you a guide to help you, nor does it give you any sort of wisdom or spiritual enlightenment. Therefore, it won't help one ascend the way Daniel did.
Also, raw knowledge alone is certainly not enough; there's a human component too (perhaps there is a need for a soul?). Elizabeth Weir found this out after failing to lead a group of human replicators to "digital ascension".
Synthesized Weir Voice: We found a suitable planet and began our work. I did what I could to help them. I tried to lead them in meditation, to teach them how to "release their burden." But it was difficult.
McKay: Let me guess, you ran into the small hiccup with the fact that you're all machines?!
Synthesized Weir Voice: Yes.
McKay: Well, as much as I'd like to say we didn't see that coming, we, you know, did.
–Stargate Atlantis, "Ghost in the Machine"
The full requirements of spiritual ascension are not fully explored, but suffice it to say, the repository of knowledge doesn't provide all of the components that are required for this.
If your brain develops to the point where it has an extremely high percentage of synaptic connection and is otherwise in a good state, you will ascend. Both Rodney McKay and Khalek nearly ascended by this method after a DNA sequencer altered their physical makeup.
Now, based on what I've extrapolated from the Ancient research, I have been able to set measurable parameters for achieving the proper mental state. Once I reach ninety six percent synaptic connection, as measured by this device ... (he points to it as Carson switches the device on and lights come on on the headband) ... all I need to do is maintain an E.E.G. frequency of zero point one to zero point nine Hertz and presto. (He clicks his fingers, then gestures skywards.) I arise to a higher plane of existence.
–Rodney McKay in Stargate Atlantis, "Tao of Rodney"
So this form of ascension is due to a physical alteration to the brain, which is not what the repository of knowledge is designed to do.
Addendum: You have to want to ascend
O'Neill has actually had the chance to ascend previously when Baal continuously tortured him to death and resurrected him. An ascended Daniel Jackson offers to help O'Neill to also ascend, but makes it clear that he has to desire it.
Okay. Let's take this one step at a time. This has to be something you want. I can't do this for you.
–Daniel Jackson in Stargate SG-1, "Abyss"
The repository of knowledge doesn't change O'Neill's wants and desires. If he has the ability to ascend, but doesn't want to, then he won't.