Recently, MFU-4l frameworks were synthesized with Mn II and Cd II central atoms, which introduced another way for tuning H2 binding enthalpies in MFU-4-type frameworks. The authors introduced Cu I to the peripheral sites of the SBU in the Mn and Cd analogues of MFU-4l and showed that the central metal can control the hydrogen binding strength at the Cu I sites of the SBU. The larger central atom in the node leads to the planarization of the copper coordination, as illustrated in Figure . This planarization affects the energy levels of dxz and dyz orbitals of Cu I , rendering π-backdonation less favorable. As a result, weakening of the binding enthalpy from -32 kJ/mol of Cu I Zn-MFU-4l to -23 kJ/mol was observed in the case of Cu I Cd II -MFU-4l, which is within the optimal range for room temperature hydrogen storage. Although the reported optimal binding strength of Cu I Cd II -MFU-4l is exciting, Cd is a toxic metal, and therefore, finding other combinations of the peripheral and central metal sites of the pentanuclear Kuratowski-type cluster using computation will guide the next target for synthetic chemists.