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Metal-free thermally activated delayed fluorescence (TADF) emitters have emerged as promising candidate materials for highly efficient and low-cost organic light-emitting diodes (OLEDs). Here, a novel acceptor 2-cyanopyrazine is selected for the construction of blue TADF molecules via computer-assisted molecular design. Both theoretical prediction and experimental photophysical data indicate a small S 1 -T 1  energy gap (Δ E  ST ) and a relative large fluorescence rate ( k  F ) in an  o -phenylene-bridged 2-cyanopyrazine/3,6-di- tert -butylcarbazole compound (TCzPZCN). The  k  F  value of 3.7 × 10 7  s −1  observed in a TCzPZCN doped film is among the highest in the TADF emitters with a Δ E  ST  smaller than 0.1 eV. Blue TADF emission is observed in a TCzPZCN doped film with a short TADF lifetime of 1.9 μs. The OLEDs using TCzPZCN as emitter exhibit a maximum external quantum efficiency (EQE) of 7.6% with low-efficiency roll-off. A sky-blue device containing a derivative of TCzPZCN achieves an improved EQE maximum of 12.2% by suppressing the non-radiative decay at T 1 .

Pyrazine-Based Blue Thermally Activated Delayed Fluorescence Materials: Combine Small Singlet–Triplet Splitting With Large Fluorescence Rate