摘要： Tremendous effort has been devoted to developing novel near-infrared (NIR) emitters and to improving the performance of NIR organic light-emitting diodes (OLEDs). Os(II) complexes are known to be an important class of NIR electroluminescent materials. However, the highest external quantum efficiency achieved so far for Os(II)-based NIR OLEDs with an emission peak wavelength exceeding 700 nm is still lower than 3%. A new series of Os(II) complexes (1–4) based on functional pyrazinyl azolate chelates and dimethyl(phenyl)phosphane ancillaries is presented. The reduced metal-to-ligand charge transfer (MLCT) transition energy gap of pyrazinyl units in the excited states results in efficient NIR emission for this class of metal complexes. Consequently, NIR OLEDs based on 1–4 show excellent device performance, among which complex 4 with a triazolate fragment gives superior performance with maximum external quantum efficiency of 11.5% at peak wavelength of 710 nm, which represent the best Os(II)-based NIR-emitting OLEDs with peak maxima exceeding 700 nm.