A molecularly tailored photosensitizer with an efficiency of 13.2% for dye-sensitized solar cells Anna Grobelny 1,2,§ , Zhongjin Shen 1,§,* , Felix T. Eickemeyer 1 , Naura F. Antariksa 1 , Szczepan Zapotoczny 2 , Shaik M. Zakeeruddin 1 , Michael Grätzel 1,* 1 Laboratory of Photonics and Interfaces (LPI), Institute of Chemical Sciences & Engineering, École Polytechnique Fédérale de Lausanne, Lausanne 1015, Switzerland, 2 Faculty of Chemistry, Jagiellonian University, Gronostajowa 2, Kraków 30-387, Poland Photosensitizers yielding superior photocurrents are crucial for copper-electrolyte-based highly efficient dye- sensitized solar cells (DSCs). Herein, we present two molecularly tailored organic sensitizers, coded ZS4 and ZS5 , through judiciously employing dithieno[3,2-b:2',3'-d]pyrrole (DTP) as the p-linker and hexyloxy-substituted diphenylquinoxaline (HPQ) or naphthalene-fused-quinoxaline (NFQ) as the auxiliary electron-accepting unit, respectively. Endowed with the HPQ acceptor, ZS4 shows more efficient electron injection and charge collection based on substantially reduced interfacial charge recombination as compared to ZS5 . As a result, ZS4 -based DSCs achieve a power conversion efficiency (PCE) of 13.2% under standard AM1.5 G sunlight, with a high short-circuit photocurrent density ( J sc ) of 16.3 mA cm -2 , an open-circuit voltage ( V oc ) of 1.05 V and a fill factor (FF) of 77.1%. Remarkably, DSCs sensitized with ZS4 exhibit an outstanding stability, retaining 95% of their initial PCE under continuous light soaking for 1000 h. To the best of our knowledge, this is a new record efficiency reported so far for copper-electrolyte-based DSCs using a single sensitizer. Our work highlights the importance of developing molecularly tailored photosensitizers for highly efficient DSCs with copper electrolyte. References 1. B. O'Regan, M. Grätzel, Nature 1991 , 353, 737. 2. L. Zhang, X. Yang, W. Wang, G. G. Gurzadyan, J. Li, X. Li, J. An, Z. Yu, H. Wang, B. Cai, A. Hagfeldt, L. Sun, ACS Energy Lett. 2019 , 4, 943. 3. Y. Cao, Y. Saygili, A. Ummadisingu, J. Teuscher, J. Luo, N. Pellet, F. Giordano, S. M. Zakeeruddin, J. E. Moser, M. Freitag, A. Hagfeldt, M. Grätzel, Nat. Commun. 2017 , 8, 15390. 4. D. Zhang, M. Stojanovic, Y. Ren, Y. Cao, F. T. Eickemeyer, E. Socie, N. Vlachopoulos, J.-E. Moser, S. M. Zakeeruddin, A. Hagfeldt, M. Grätzel, Nat. Commun. 2021 , 12, 1777. 5. W. Zhang, Y. Wu, H. W. Bahng, Y. Cao, C. Yi, Y. Saygili, J. Luo, Y. Liu, L. Kavan, J.-E. Moser, A. Hagfeldt, H. Tian, S. M. Zakeeruddin, W.-H. Zhu, M. Grätzel, Energy Environ. Sci. 2018 , 11, 1779. 6. H. Jiang, Y. Ren, W. Zhang, Y. Wu, E. C. Socie, B. I. Carlsen, J.-E. Moser, H. Tian, S. M. Zakeeruddin, W.-H. Zhu, M. Grätzel, Angew. Chem. Int. Ed. 2020 , 59, 9324. 7. P. Gao, H. N. Tsao, J. Teuscher, M. Grätzel, Chin. Chem. Lett. 2018 , 29, 289.
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