Supporting Information

Table S1.The lattice parameters of TM3(HITP)2 MOFs. Table S2. The adsorption energy of nitrogen adsorbed by TM3(HITP)2 MOFs, the Gibbs free energy of the first hydrogenation and the Gibbs free energy of the sixth hydrogenation. Table S3. Charge transfer of metal atoms and electronegativity of transition metals before and after nitrogen adsorption by TM3(HITP)2MOFs. Figure S1. The distribution of (a) and (b) represents the charge transfer diagram of moiety1, moiety2, and moiety3 of Mo3(HITP)2 and Os3(HITP)2 along the distal pathway. Figure S2. The relationship between UL and ΔQTM•XTM•4XS in TM3C24N6X12 MOF. Figure S3. Gibbs free energy changes along the alternate pathway of NRR in Mo3(HITP)2 (a) and Os3(HITP)2 (b).