Twice a day should be plenty - most cats in the wild only eat once a day, and it's a mouse or some other small critter, so they're not going to starve if they don't get three square meals. Putting it down and taking it back up regardless of whether they've eaten it or not is the preferred method - free-feeding tends to lead to obesity. You can train cats to some extent, but it usually takes more energy and more consistency than most people are willing to put in.
The real issue isn't the cats but your respect for your wife's feelings. If the cats are very important to her, what does it matter to you whether they're fed three or two times a day? It is better for their health to be fed fewer times, and to have to eat it when it's put down, but in the long run, what's more important to you: being right, or having your wife be happy?
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"If ten million people believe a foolish thing, it is still a foolish thing."
- Anatole France
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