So while this post can be fairly accused of being entirely self-serving, I did want to weigh in on why I think a Cataloging background makes one a better Interlibrary Loan staffer. The simplest reason being that your primary tool is OCLC/Worldcat which is the worldwide database used by libraries to report their holdings to all other libraries, with a heavy emphasis on the Anglo-American, English-speaking parts of the world. I don't have experience with ILLiad or other ILL interfaces. Our main interface in Texas is called NRE, or simply "Navigator". And while it is possible to use Navigator to search OCLC/Worldcat indirectly, we've found in actual practice it pays to subscribe to both NRE *and* OCLC/WorldCat for maximum coverage. There are different things each interface does better than the other.
But the basis of all records in NRE and OCLC/WorldCat is the bibliographic record. A cataloger understands from experience how these are constructed, why they're constructed the way they are, etc. We have an almost intuitive understanding of how search functions work, why books are cataloged the way they are, and also that duplicate records exist sometimes and it can be fruitful to pull from multiple sources. There are ways to "tweak" ILL requests for maximum coverage if you understand these nuances and improve the chances of your patron actually getting the book that they want and getting it to them in a timely manner.
For academic journal requests we nearly always use OCLC/WorldCat as the preferred search interface. It is easier to facilitate a request using Article Exchange on that platform. Moreover, I usually try to select the digital ISSN whenever possible. While it is technically possible to scan hard-copy as a PDF and send out that way, I prefer not to put that burden on potential lenders if I can help it. I do plenty of that myself and know what a pain it can be. If I can download and send an article completely digitally then I certainly want to do that in favor of manually creating a scanned PDF.
It is an experienced cataloger that knows about ISSN's and will search relentlessly to track them down. I am damn good at this and that's why my ILL partner nearly always defers to me for these kinds of searches. An ISSN is a more precise search than a clumsy title search, and avoids the difficulty of journal name changes, etc.
It's hard to articulate in a comprehensive way why ex-catalogers are good at ILL, just that it shapes your approach to and understanding of bibliographic information in ways that non-catalogers don't have naturally. The job conditions you to be aware of these finer points of bibliographic record construction and dissemination. It makes a good fall-back position for anyone deciding to leave the realm of library cataloging and change directions.
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