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It does not sound to me as if your machine spec is a problem. I can understand why the NAS might slow down Calibre2Opds, but not why it would make it fail to run. I use Calibre2Opds against my NAS with a much bigger library. In my case Calibre2Opds can take a few hours to complete the run, but I do not have the problem you report of it failing to run.
In terms of speeding Calibre up, you might want to look for the Calibre-Portable.bat file that is held in the resources sub-folder of the Calibre install location. It shows you how you can control where all the Calibre files are located. I use it to keep the calibre metadata.db file on my local hard disk with all the Book files on the NAS. I then periodically copy the metadata.db file into the NAS Calibre library location.
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