(a) DFT-predicted crystal structures of e-2-OH–Mg2(dobpdc) with oxygen-bound e-2-OH (left) and CO2-inserted e-2-OH–Mg2(dobpdc) (right). (b) Predicted structure of CO2-inserted e-2-OH–Mg2(dobpdc), as viewed along the pore wall. (c) View down the c-axis of the predicted structure of CO2-inserted e-2-OH–Mg2(dobpdc). All structures were calculated as described in Section 17 of the Supporting Information. Grey, red, blue, white, and green spheres represent C, O, N, H, and Mg atoms, respectively. (d) Proposed CO2 adsorption mechanism for alcoholamine-appended Mg2(dobpdc) involving hydrogen bond-stabilized carbamic acid chains.