A new strategy of platinum(II) complexation is developed to regulate the crystallinity and molecular packing of polynitrogen heterocyclic polymers, optimize the morphology of the active blends, and improve the efficiency of the resulting nonfullerene polymer solar cells (NF-PSCs). The newly designed s-tetrazine (s-TZ)-containing copolymer of PSFTZ (4,8-bis(5-((2-butyloctyl)thio)-4-fluorothiophen-2-yl)benzo[1,2-b:4,5-b']dithiophene-alt-3,6-bis(4-octylthiophen-2-yl)-1,2,4,5-tetrazine) has a strong aggregation property, which results in serious phase separation and large domains when blending with Y6 ((2,2'-((2Z,2'Z)-((12,13-bis(2-ethylhexyl)-3,9-diundecyl-12,13-dihydro-[1,2,5]thiadiazolo[3,4-e]thieno[2″,3″:4',5']thieno[2',3':4,5]pyrrolo[3,2-g]thieno[2',3':4,5]thieno[3,2-b]indole-2,10-diyl)bis(methanylylidene))bis(5,6-difluoro-3-oxo-2,3-dihydro-1H-indene-2,1-diylidene))dimalononitrile)), and produces a power-conversion efficiency (PCE) of 13.03%. By adding small amount of Pt(Ph) (DMSO) (Ph, phenyl and DMSO, dimethyl sulfoxide), platinum(II) complexation would occur between Pt(Ph) (DMSO) and PSFTZ. The bulky benzene ring on the platinum(II) complex increases the steric hindrance along the polymer main chain, inhibits the polymer aggregation strength, regulates the phase separation, optimizes the morphology, and thus improves the efficiency to 16.35% in the resulting devices. 16.35% is the highest efficiency for single-junction PSCs reported so far.
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