By definition this setup would not be a closed-loop design, but I assume you're talking about the Ecotech mode called closed-loop. That said - I see no reason why it wouldn't work as long as your plumbing from the overflow is large enough to support the GPH you will need to get the flow you want from the pump. Keep in mind you will have head pressure when not in a true closed-loop design so your max GPH will need to be calculated from the max 3100GPH rating.
Personally, I used the L1 in a closed loop and while it worked, I eventually took it down since I didn't see the benefit of enough extra flow I wanted from the setup. One advantage you should see (that I didn't) from using it as an extra return pump vs a closed-loop is the lack of debris (think sand) getting into the pump and causing noise. I even had the return line mounted high in the tank to reduce this issue, but I was always having to mess with it to clear sand out of it... Very annoying! With the inlet in the sump, you will not have this issue.
One other thing to consider is how silent your overflow is. If you have your overflow tuned to be quite, you will likely have a hard time keeping it silent since the pump will be constantly changing the amount of GPH over the overflow. A true closed-loop will not do this since the water doesn't go over the overflow.
Final thoughts... With 2" acrylic I assuming the tank is huge. Do you want the closed-loop to have a cleaner look, or are you OK with cables in the tank? When I compare a powerhead (or wavebox) to the L2, I can achieve the same amount of flow with fewer watts. depending on placement, I would consider building mounts that would work with powerheads for the walls of the tank or hide the powerheads in the rockwork if you can hide the cables (see below). Just my .02 cents from using a closed-loop in the past.
Tunze Stream rock
Hi-Tech für Aquaristik
www.tunze.com