Fine Tuning of Donor-Acceptor Structures in Fused-Carbazole Containing Thermally Activated Delayed Fluorescence Materials towards High-Efficiency OLEDs

Comprehensive Summary Conjugated fused-ring structures have attracted extensive attention due to their high molecular rigidity to restrain excited-state relaxation and non-radiative decay,and further to enhance the luminance efficiency for emissive materials.Herein,we develop a series of donor-acceptor type thermally activated delayed fluorescence(TADF)emitters by introducing fused-ring 5H-benzofuro[3,2-c]carbazole(32BFCz)as electron donating unit.Through optimizing the numbers and structure of donor and acceptor moieties,three compounds named 32BFCzA,mCF3BFCzOXD and dCF3BFCzOXD are designed,which are composed by mono-32BFCz/trifluoromethylpicolinonitrile,penta-BFCz/3-(trifluoromethyl)phenyl)-1,3,4-oxadiazol-2-yl)benzene and penta-32BFCz/3,5-bis(trifluoromethyl)phenyl)-1,3,4-oxadiazol-2-yl)benzene as donor/acceptor groups,respectively.

Molecular engineering on all ortho-linked carbazole/oxadiazole hybrids toward highly-efficient thermally activated delayed fluorescence materials in OLEDs

The highest efficiency thermally activated delayed fluorescence(TADF)emitters in OLEDs are mostly based on twisted donor/acceptor(D/A)type organic molecules.Herein,we report the rational molecular design on twisted all ortho-linked carbazole/oxadiazole(Cz/OXD)hybrids with tunable D-A interactions by adjusting the numbers of donor/acceptor units and electron-donating abilities.Singlet-triplet energy bandgaps(ΔEST)are facilely tuned from^0.4,0.15 to^0 eV in D-A,D-A-D to A-D-A type compounds.This variation correlates well with triplet-excited-state frontier orbital spatial separation efficiency.NonTADF feature with solid state photoluminescence quantum yield(PLQY)<10%is observed in D-A type 2CzOXD and D-A-D type 4CzOXD.Owing to the extremely lowΔEST for efficient reverse intersystem crossing,strong TADF with PLQY of 71%-92%is achieved in A-D-A type 4CzDOXD and 4tCzDOXD.High external quantum efficiency from 19.4%to 22.6%is achieved in A-D-A typed 4CzDOXD and 4tCzDOXD.

Phosphide-oxide honeycomb-like heterostructure CoP@CoMoO4/CC for enhanced hydrogen evolution reaction in alkaline solution

The design and construction of effective and stable hydrogen evolution reaction(HER)catalysts represent the key to obtaining hydrogen energy economically.Transition metal phosphides(TMPs)have attracted considerable attention due to their unique catalytic mechanism,which is similar to hydrogenase.However,single-phase TMPs remain limited by their low activity and weak stability in alkaline solutions.In this work,CoP@CoMoO4 nanosheets with phosphide and oxide heterostructure were synthesized on carbon cloth(CC)through hydrothermal method and subsequently reacted with red phosphorus in a tube furnace.The outstanding synergy between CoP and CoMoO4 enhanced the HER activity and stability in alkaline solution.The CoP@CoMoO4/CC heterostructure exhibited excellent HER activity with a low overpotential of 89 mV at 10 mA cm^-2 with Tafel slope of 69 mV dec^-1,and outstanding stability when compared with single-phase phosphides.Our present research provides a new approach for the preparation of inexpensive,highly active,and highly durable phosphorus-based catalyst for HER.