Using existing cooling towers to capture atmospheric CO2 seems like a much better idea than using energy to otherwise pump tonnes of air through a process. However, I can't help wonder whether it is better than capturing the exhaust emissions (primarily CO2 and H20) directly from the exhaust gasses, before they are released to the atmosphere.
Removing emissions from smokestacks is critical to ensuring we can stop dumping waste into the sky, but we are at the point now where we need scalable, low-cost processes to pull carbon out of the atmosphere.
So, we need to definitely do what you're suggesting and capture all emissions from as many smokestacks as possible until we've fully transitioned to a clean grid. And, we also need to begin pulling CO2 out of the atmosphere.