OK. Fixed... many thanks to this post for clearing up a few details.
To eliminate the 503 errors required 3 different config changes:
machine.config:
<configuration>
...
<system.web>
...
<processModel enable="true" requestQueueLimit="100000"/>
IIS Manager > ApplicationPools > Advanced Settings
Queue Length : 65535
and finally (the missing piece of the puzzle), the command line:
appcmd.exe set config /section:serverRuntime /appConcurrentRequestLimit:100000
The web.config setting mentioned in the main post was irrelevant.
10000 concurrent connections, no problems. Thanks for help!