Your understanding of what's happening is not.
Deep buried rocks are not in some minimum energy state with respect to the atmosphere. As you can readily see from the rapid chemical changes that happen to lava flows when exposed to the atmosphere - most visibly, the oxidation of FeO to Fe2O3. Not only is deep buried rock not exposed to the atmosphere, but the thermodynamic equlibria are also different under their different temperatures and pressures. In said rocks, calcium and magnesium oxide and hydroxide - as with a typical basaltic lava flow - like 15%-ish of their mass in basalt like that under Hellisheiði - can bind with CO2 to form carbonates. This happens naturally (calcite, aragonite, magnesite, dolomite, etc), and we can induce it artificially as well by providing the CO2. And it most demonstrably works - on surprisingly short timescales, too. But you need the right strata to be present, and you need wells down to them.
If you don't believe me, quick question: you know what quicklime is? You know how you make it? You take limestone (calcium carbonate), and you apply heat to it to decompose it to calcium oxide and carbon dioxide. You have to input energy, even at surface conditions, let alone under the pressure at depth, to turn it into calcium oxide. It's more thermodynamically favourable for it to be in the state of calcium carbonate than it is for it to be in the state of calcium oxide plus CO2.
You can potentially see this in your own house. Ever seen a concrete slab that's started to burst out, exposing the rebar? Do you know why that happens? Carbonation. Steel in the high-pH environment of concrete is rendered passive; oxidation rates are almost nonexistent. However, concrete contains calcium hydroxide. This slowly reacts with carbon dioxide from the atmosphere to form, again, calcium carbonate. Because the very cement in the concrete was itself made by applying energy to drive the CO2 off, and it's now returning to its earlier state. As the carbonated layer gets deeper and deeper, it eventually reaches the steel; the pH drops, the steel is no longer protected, starts to rust, expands, and the concrete spalls out.
Thermodynamic equilibria vary with temperature and pressure - that is, a reaction may go in one direction in certain conditions, but the opposite direction in others. For example, driving CO2 off calcium carbonate with heat to make quicklime, cooling it down, then react with water to make calcium hydroxide, which slowly reabsorbs CO2; at elevated temperature at 1 ATM, the opposite reaction was favoured to at lower temperatures at 1 ATM. The balance is complex, because heat may favour a given reaction but pressure may disfavour it, or vice versa; it all depends on the specifics.
Deep rocks are simply not in thermodynamic equilibrium with the surface. Period. Because this is a system with huge differences in temperature and pressure with depth, changing their thermodynamic equilibria as matter cycles both up and down through the crust and mantle. Gas commonly escapes during these changes, rising to the surface and is lost. Rocks that would slowly absorb CO2 (or oxygen) if they were on the surface to exist in a non-reacted - but reactive - state, because the things they could react with simply don't exist there. A situation you can remedy by supplying said CO2.
Do you understand now?
it would reduce atmospheric carbon more if this green energy was used to power whatever we want to power
This green energy is located in Iceland, a remote island country where essentially 100% of all electricity consumption is already from clean energy. The only way we can export energy (barring the megaengineering project of the world's longest subsea power cable, by huge margins) is to do energy-intensive industrial activity here. For example, there's not a single bauxite mine in the country, but we're a major alumium producer, importing bauxite and exporting the metal, and in effect, exporting its embodied power. It would be more efficient to do the processing closer to ore production, but the power is here, not there, and we can't just send it there.