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000454549 1001_ $$0P:(DE-HGF)0$$aYao, Zhaoyang$$b0
000454549 245__ $$aConformational and Compositional Tuning of Phenanthrocarbazole-Based Dopant-Free Hole-Transport Polymers Boosting the Performance of Perovskite Solar Cells
000454549 260__ $$aWashington, DC$$bAmerican Chemical Society$$c2020
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000454549 520__ $$aConjugated polymers are regarded as promising candidates for dopant-free hole-transport materials (HTMs) in efficient and stable perovskite solar cells (PSCs). Thus far, the vast majority of polymeric HTMs feature structurally complicated benzo[1,2-b:4,5-b’]dithiophene (BDT) analogs and electron-withdrawing heterocycles, forming a strong donor–acceptor (D–A) structure. Herein, a new class of phenanthrocarbazole (PC)-based polymeric HTMs (PC1, PC2, and PC3) has been synthesized by inserting a PC unit into a polymeric thiophene or selenophene chain with the aim of enhancing the $π–π$ stacking of adjacent polymer chains and also to efficiently interact with the perovskite surface through the broad and planar conjugated backbone of the PC. Suitable energy levels, excellent thermostability, and humidity resistivity together with remarkable photoelectric properties are obtained via meticulously tuning the conformation and elemental composition of the polymers. As a result, PSCs containing PC3 as dopant-free HTM show a stabilized power conversion efficiency (PCE) of 20.8% and significantly enhanced longevity, rendering one of the best types of PSCs based on dopant-free HTMs. Subsequent experimental and theoretical studies reveal that the planar conformation of the polymers contributes to an ordered and face-on stacking of the polymer chains. Furthermore, introduction of the “Lewis soft” selenium atom can passivate surface trap sites of perovskite films by Pb–Se interaction and facilitate the interfacial charge separation significantly. This work reveals the guiding principles for rational design of dopant-free polymeric HTMs and also inspires rational exploration of small molecular HTMs.
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000454549 7001_ $$00000-0002-2789-7714$$aZhang, Fuguo$$b1
000454549 7001_ $$0P:(DE-HGF)0$$aGuo, Yaxiao$$b2
000454549 7001_ $$0P:(DE-HGF)0$$aWu, Heng$$b3
000454549 7001_ $$0P:(DE-HGF)0$$aHe, Lanlan$$b4
000454549 7001_ $$0P:(DE-HGF)0$$aLiu, Zhou$$b5
000454549 7001_ $$0P:(DE-HGF)0$$aCai, Bin$$b6
000454549 7001_ $$0P:(DE-HGF)0$$aGuo, Yu$$b7
000454549 7001_ $$0P:(DE-H253)PIP1021935$$aBrett, Calvin$$b8
000454549 7001_ $$0P:(DE-H253)PIP1027114$$aLi, Yuanyuan$$b9
000454549 7001_ $$0P:(DE-HGF)0$$aSrambickal, Chinmaya Venugopal$$b10
000454549 7001_ $$00000-0002-3035-4163$$aYang, Xichuan$$b11
000454549 7001_ $$0P:(DE-H253)PIP1080777$$aChen, Gang$$b12
000454549 7001_ $$00000-0003-3200-0374$$aWidengren, Jerker$$b13
000454549 7001_ $$0P:(DE-HGF)0$$aLiu, Dianyi$$b14
000454549 7001_ $$00000-0002-4782-4969$$aGardner, James M.$$b15
000454549 7001_ $$00000-0002-0168-2942$$aKloo, Lars$$b16
000454549 7001_ $$0P:(DE-H253)PIP1083782$$aSun, Licheng$$b17$$eCorresponding author
000454549 773__ $$0PERI:(DE-600)1472210-0$$a10.1021/jacs.0c08352$$gVol. 142, no. 41, p. 17681 - 17692$$n41$$p17681 - 17692$$tJournal of the American Chemical Society$$v142$$x1520-5126$$y2020
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