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In this work, a large excess of electrostatic repulsion, arising from the axial ligands, over that from the equatorial ligands is taken as the design strategy for high performance pentagonal bipyramidal (PBP) DyIII single-ion magnets (SIMs).

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It is a tremendous challenge to prepare solvent-free dense energetic metal-organic frameworks (EMOFs), hence also to improve their stability and energetic performance. In this study, based on in situ microcalorimetry, an interpenetrating EMOF without solvent molecules, [Cu(tztr)] (1, Htztr = 3-(tetrazol-5-yl)triazole) was obtained, possessing high stability (T = 360 °C) and outstanding energetic properties (ΔH = 7.53 kcal cm, D = 8.429 km s, P = 40.02 GPa).

Redox‐active conjugated microporous polymers (RCMPs) have received remarkable interest in electrochemical energy‐storage systems in view of their porous structure and tunable redox nature. This work presents an effective strategy to construct RCMPs with bipolar and double redox‐active centers by integrating copper (II) tetraaminephthalocyanine (CuTAPc) and 1,4,5,8‐naphthalenetetracarboxylic dianhydride (NTCDA) units into the RCMPs (CuPcNA‐CMP). As expected, CuPcNA‐CMP has potential application in the half cells of dual‐ion batteries (lithium based DIBs, LDIBs), asymmetric DIBs (graphite based DIBs, ADIBs), and symmetric DIBs (all organic DIBs, SDIBs). Among them, LDIBs show a high reversible capacity (202.4 mAh g−1 at 0.2 A g−1) and excellent rate capability (86.1 mAh g−1 at 5 A g−1). And ADIBs also show a high reversible capacity (245.3 mAh g−1 at 0.1 A g−1), long cycle stability with capacity retention of 89% after 500 cycles, and good rate performance (125.1 mAh g−1 at 5 A g−1). In addition, SDIBs show high initial charge/discharge capacities of 269.4/198.5 mAh g−1 at 0.05 A g−1 and a high cell voltage of 2.5 V. Meanwhile, the mechanism of CuPcNA‐CMP on hosting both anions (PF6−) and cations (Li+) is investigated by detailed experimental analysis and density functional theory studies.

A novel two-dimensional (2D) coordination polymer, [Co(ppad)2]n (1), resulted from the assembly of Co(II) ions based on a versatile ligand termed N(3)-(3-pyridoyl)-3-pyridinecarboxamidrazone. Alternating/direct-current magnetic studies of compound 1 indicate that the spatially separated high-spin Co(II) ions act as single-ion magnets (SIMs). The present work represents the first case of a 2D Co(II)-based SIM composed of a monocomponent organic spacer.

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