Emails won't send via 3G if primary server is on

I have a natty problem, I have 6 email accounts set up on iPhone 5S & iPad Air. No issues sending or receiving emails on either device via wifi but cannot send via 3G/4G unless I first go into settings and turn off Primary Outgoing Mail Server - relay.plus.net (and sometimes subsequent servers) only when I've switched it off will it send normally using smtp.o2.co.uk. The iPhone as stated at bottom of outgoing server list says "If Mail is unsuccessful using primary server, it will try the other SMTP servers in succession" unfortunately I have the primary (relay.plus.net) followed by a further 7 relay.plus.net, then 2 x smtp.gmail.com, then smtp.talktalk.net, mail.btinternet.com then lastly smtp.o2.co.uk. No idea why I have so many plus.net servers nor 2 gmail servers. Don't want to set O2 as primary server incase it then fails to send using wifi.
Any assistance would be of great help please.

Hi Modular747 thanks for reply but that's not the case, after I've turned off the primary server, any mail gets sent fine on either account via 3G/4G but sits as unable to send in outgoing box if primary server is switched on.

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