Multiple-Asymmetric Molecular Engineering Enables Regioregular Selenium-Substituted Acceptor with High Efficiency and Ultra-low Energy Loss in Binary Organic Solar Cells
Dr. Can Yang
Key Laboratory of Cluster Science of Ministry of Education, Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing, 100081 China
Both authors contributed equally to this work.
Search for more papers by this authorDr. Yuan Gao
The Institute for Advanced Studies, Wuhan University, Wuhan, 430072 China
Both authors contributed equally to this work.
Search for more papers by this authorHeng Zhang
Key Laboratory of Cluster Science of Ministry of Education, Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing, 100081 China
Search for more papers by this authorDr. Ze-Fan Yao
College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871 China
Search for more papers by this authorEr-Long Li
Key Laboratory of Cluster Science of Ministry of Education, Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing, 100081 China
Search for more papers by this authorHong-Hai Guan
Key Laboratory of Cluster Science of Ministry of Education, Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing, 100081 China
Search for more papers by this authorHong-Fu Zhi
Key Laboratory of Cluster Science of Ministry of Education, Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing, 100081 China
Search for more papers by this authorQuan Yuan
Key Laboratory of Cluster Science of Ministry of Education, Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing, 100081 China
Search for more papers by this authorDr. Min Hun Jee
Department of Chemistry, Korea University, Seoul, 136-713 Republic of Korea
Search for more papers by this authorProf. Han Young Woo
Department of Chemistry, Korea University, Seoul, 136-713 Republic of Korea
Search for more papers by this authorCorresponding Author
Prof. Jie Min
The Institute for Advanced Studies, Wuhan University, Wuhan, 430072 China
E-mail: [email protected]; [email protected]
Search for more papers by this authorCorresponding Author
Prof. Jin-Liang Wang
Key Laboratory of Cluster Science of Ministry of Education, Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing, 100081 China
E-mail: [email protected]; [email protected]
Search for more papers by this authorDr. Can Yang
Key Laboratory of Cluster Science of Ministry of Education, Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing, 100081 China
Both authors contributed equally to this work.
Search for more papers by this authorDr. Yuan Gao
The Institute for Advanced Studies, Wuhan University, Wuhan, 430072 China
Both authors contributed equally to this work.
Search for more papers by this authorHeng Zhang
Key Laboratory of Cluster Science of Ministry of Education, Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing, 100081 China
Search for more papers by this authorDr. Ze-Fan Yao
College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871 China
Search for more papers by this authorEr-Long Li
Key Laboratory of Cluster Science of Ministry of Education, Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing, 100081 China
Search for more papers by this authorHong-Hai Guan
Key Laboratory of Cluster Science of Ministry of Education, Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing, 100081 China
Search for more papers by this authorHong-Fu Zhi
Key Laboratory of Cluster Science of Ministry of Education, Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing, 100081 China
Search for more papers by this authorQuan Yuan
Key Laboratory of Cluster Science of Ministry of Education, Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing, 100081 China
Search for more papers by this authorDr. Min Hun Jee
Department of Chemistry, Korea University, Seoul, 136-713 Republic of Korea
Search for more papers by this authorProf. Han Young Woo
Department of Chemistry, Korea University, Seoul, 136-713 Republic of Korea
Search for more papers by this authorCorresponding Author
Prof. Jie Min
The Institute for Advanced Studies, Wuhan University, Wuhan, 430072 China
E-mail: [email protected]; [email protected]
Search for more papers by this authorCorresponding Author
Prof. Jin-Liang Wang
Key Laboratory of Cluster Science of Ministry of Education, Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing, 100081 China
E-mail: [email protected]; [email protected]
Search for more papers by this authorGraphical Abstract
The synergistic strategies of the double asymmetric core and symmetric/asymmetric terminal engineering are applied to develop multiple-asymmetric acceptors. By delicately tuning the number and position of peripheral F and Cl atoms, the regioregular triple-asymmetric TASe-2F2Cl-based binary OSCs yield the first-class efficiency of 19.32% and ultralow nonradiative recombination energy loss (ΔE3) among selenium-substituted acceptors.
Abstract
Asymmetric molecular engineering is utilized for developing efficient small molecular acceptors (SMAs), whereas adopting multiple asymmetric strategies at the terminals, side chains, and cores of efficient SMAs remains a challenge, and effects on reducing energy loss (Eloss) have been rarely investigation. Herein, four regioregular multiple-asymmetric SMAs (DASe-4F, DASe-4Cl, TASe-2Cl2F, and TASe-2F2Cl) are constructed by delicately manipulating the number and position of F and Cl on end groups. Triple-asymmetric TASe-2F2Cl not only exhibits a unique and most compact 3D network crystal stacking structure but also possesses excellent crystallinity and electron mobility in neat film. Surprisingly, the PM1:TASe-2F2Cl-based binary organic solar cells (OSCs) yield a champion power conversion efficiencies (PCEs) of 19.32%, surpassing the PCE of 18.27%, 17.25%, and 16.30% for DASe-4F, DASe-4Cl, and TASe-2Cl2F-based devices, which attributed to the optimized blend morphology with proper phase separation and more ordered intermolecular stacking and excellent charge transport. Notably, the champion PCE of 19.32% with ultralow nonradiative recombination energy loss (ΔE3) of 0.179 eV marks a record-breaking result for selenium-containing SMAs in binary OSCs. Our innovative multiple-asymmetric molecular engineering of precisely modulating the number and position of fluorinated/chlorinated end groups is an effective strategy for obtaining highly-efficient and minimal ΔE3 of selenium-substituted SMAs-based binary OSCs simultaneously.
Conflict of Interests
The authors declare no conflict of interest.
Open Research
Data Availability Statement
The data that support the findings of this study are available in Supporting Information of this article.
Supporting Information
| Filename | Description |
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| anie202506795-sup-0001-SuppMat.docx14.4 MB | Supporting Information |
| anie202506795-sup-0002-SuppMat.zip863.5 KB | Supporting Information |
Please note: The publisher is not responsible for the content or functionality of any supporting information supplied by the authors. Any queries (other than missing content) should be directed to the corresponding author for the article.
References
- 1Z. Wang, D. Zhang, L. Yang, O. Allam, Y. Gao, Y. Su, M. Xu, S. Mo, Q. Wu, Z. Wang, J. Liu, J. He, R. Li, X. Jia, Z. Li, L. Yang, M. D. Weber, Y. Yu, X. Zhang, T. J. Marks, N. Stingelin, J. Kacher, S. S. Jang, A. Facchetti, M. Shao, Science 2025, 387, 381–387.
- 2G. Zhang, F. R. Lin, F. Qi, T. Heumüller, A. Distler, H.-J. Egelhaaf, N. Li, P. C. Y. Chow, C. J. Brabec, A. K. Y. Jen, H.-L. Yip, Chem. Rev. 2022, 122, 14180–14274.
- 3R. Zeng, J. Deng, X. Xue, S. Tan, L. Kan, Y. Lin, W. Zhong, L. Zhu, F. Han, Y. Zhou, X. Gao, M. Zhang, Y. Zhang, S. Xu, F. Liu, Angew. Chem. Int. Ed. 2025, 64, e202420453.
- 4S.-Y. Shi, C. Yang, X. Xu, Z.-X. Liu, W. Duan, X.-X. Chen, Z. Lu, H. Zhou, Z.-P. Yu, C.-Z. Li, Angew. Chem. Int. Ed. 2024, 64, e202415994.
- 5X. Zhang, H. Gao, Y. Kan, X. Wang, W. Zhang, K. Zhou, H. Xu, L. Ye, R. Yang, Y. Yang, X. Hao, Y. Sun, K. Gao, Angew. Chem. Int. Ed. 2025, 64, e202415583.
- 6W. Zhou, J. Liu, J. Xie, S. You, J. Deng, F. Yu, S. Y. Jeong, H. Y. Woo, F. Wu, L. Chen, Angew. Chem. Int. Ed. 2025, 64, e202415141.
- 7W. Liu, H. Zhang, S. Liang, T. Wang, S. He, Y. Hu, R. Zhang, H. Ning, J. Ren, A. Bakulin, F. Gao, J. Yuan, Y. Zou, Angew. Chem. Int. Ed. 2023, 62, e202311645.
- 8H. Fu, M. Zhang, Y. Zhang, Q. Wang, Z. Xu, Q. Zhou, Z. Li, Y. Bai, Y. Li, Z.-G. Zhang, Angew. Chem. Int. Ed. 2023, 62, e202306303.
- 9J. Wu, Z. Ling, L. R. Franco, S. Y. Jeong, Z. Genene, J. Mena, S. Chen, C. Chen, C. M. Araujo, C. F. N. Marchiori, J. Kimpel, X. Chang, F. H. Isikgor, Q. Chen, H. Faber, Y. Han, F. Laquai, M. Zhang, H. Y. Woo, D. Yu, T. D. Anthopoulos, E. Wang, Angew. Chem. Int. Ed. 2023, 62, e202302888.
- 10S. Ma, B. Li, S. Gong, J. Wang, B. Liu, S. Young Jeong, X. Chen, H. Young Woo, K. Feng, X. Guo, Angew. Chem. Int. Ed. 2023, 62, e202308306.
- 11M. An, Q. Liu, S. Y. Jeong, B. Liu, E. Huang, Q. Liang, H. Li, G. Zhang, H. Y. Woo, L. Niu, X. Guo, H. Sun, Angew. Chem. Int. Ed. 2024, 63, e202410498.
- 12H. Iwasaki, K. Yamanaka, Y. Sato, T. Mikie, M. Saito, H. Ohkita, I. Osaka, Angew. Chem. Int. Ed. 2024, 63, e202409814.
- 13Z. Wang, S. Zhu, X. Peng, S. Luo, W. Liang, Z. Zhang, Y. Dou, G. Zhang, S. Chen, H. Hu, Y. Chen, Angew. Chem. Int. Ed. 2025, 64, e202412903.
- 14J. Chen, D. Li, M. Su, Y. Xiao, H. Chen, M. Lin, X. Qiao, L. Dang, X.-C. Huang, F. He, Q. Wu, Angew. Chem. Int. Ed. 2023, 62, e202215930.
- 15Q. Jiang, X. Yuan, Y. Li, Y. Luo, J. Zhu, F. Zhao, Y. Zhang, W. Wei, H. Feng, H. Li, J. Wu, Z. Ma, Z. Tang, F. Huang, Y. Cao, C. Duan, Angew. Chem. Int. Ed. 2025, 64, e202416883.
- 16T. Lin, Y. Hai, Y. Luo, L. Feng, T. Jia, J. Wu, R. Ma, T. A. Dela Peña, Y. Li, Z. Xing, M. Li, M. Wang, B. Xiao, K. S. Wong, S. Liu, G. Li, Adv. Mater. 2024, 36, 2312311.
- 17X. Chen, M. Chen, J. Liang, H. Liu, X. Xie, L. Zhang, D. Ma, J. Chen, Adv. Mater. 2024, 36, 2313074.
- 18T. Duan, J. Wang, W. Shi, Y. Li, K. Tu, X. Bi, C. Zhong, J. Lv, K. Yang, Z. Xiao, B. Kan, Y. Zhao, Angew. Chem. Int. Ed. 2024, 63, e202407890.
- 19W. Liu, W. Guo, L. Fu, Y. Duan, G. Han, J. Gao, H. Liu, Y. Wang, Z. Ma, Y. Liu, Angew. Chem. Int. Ed. 2025, 64, e202416751.
- 20X. Gu, R. Zeng, Y. Hou, N. Yu, J. Qiao, H. Li, Y. Wei, T. He, J. Zhu, J. Deng, S. Tan, C.'e. Zhang, Y. Cai, G. Long, X. Hao, Z. Tang, F. Liu, X. Zhang, H. Huang, Angew. Chem. Int. Ed. 2024, 63, e202407355.
- 21X. Zheng, X. Jiang, W. Liu, C. Cao, N. Wei, Z. Wei, L. Zhang, H. Wu, A. Zhang, C. Li, Y. Liu, H. Lu, X. Xu, Z. Tang, Z. Bo, Angew. Chem. Int. Ed. 2024, 63, e202412854.
- 22K. Wang, S. Jinnai, T. Urakami, H. Sato, M. Higashi, S. Tsujimura, Y. Kobori, R. Adachi, A. Yamakata, Y. Ie, Angew. Chem. Int. Ed. 2024, 63, e202412691.
- 23Y. Che, M. R. Niazi, Q. Chan, P. Ghamari, T. Yu, C. Ruchlin, H. Yu, H. Yan, D. Ma, S. S. Xiao, R. Izquierdo, D. F. Perepichka, Angew. Chem. Int. Ed. 2023, 62, e202309003.
- 24J. Zhou, D. He, Y. Li, F. Huang, J. Zhang, C. Zhang, Y. Yuan, Y. Lin, C. Wang, F. Zhao, Adv. Mater. 2023, 35, 2207336.
- 25J. Wang, X. Zhan, Acc. Chem. Res. 2021, 54, 132–143.
- 26F. Liu, Y. Jiang, R. Xu, W. Su, S. Wang, Y. Zhang, K. Liu, S. Xu, W. Zhang, Y. Yi, W. Ma, X. Zhu, Angew. Chem. Int. Ed. 2024, 63, e202313791.
- 27X. Wu, Y. Gong, X. Li, S. Qin, H. He, Z. Chen, T. Liang, C. Wang, D. Deng, Z. Bi, W. Ma, L. Meng, Y. Li, Angew. Chem. Int. Ed. 2025, 64, e202416016.
- 28H. Fang, Q. Chen, Y. Lin, X. Xu, J. Wang, M. Li, C. Xiao, C. R. McNeill, Z. Tang, Z. Lu, W. Li, Angew. Chem. Int. Ed. 2025, 64, e202417951.
- 29J. Ren, S. Zhang, Z. Chen, T. Zhang, J. Qiao, J. Wang, L. Ma, Y. Xiao, Z. Li, J. Wang, X. Hao, J. Hou, Angew. Chem. Int. Ed. 2024, 63, e202406153.
- 30H. Lu, D. Li, W. Liu, G. Ran, H. Wu, N. Wei, Z. Tang, Y. Liu, W. Zhang, Z. Bo, Angew. Chem. Int. Ed. 2024, 63, e202407007.
- 31Y. Cho, Z. Sun, G. Li, D. Zhang, S. Yang, T. J. Marks, C. Yang, A. Facchetti, J. Am. Chem. Soc. 2025, 147, 758–769.
- 32J. Ren, J. Wang, J. Qiao, Z. Chen, X. Hao, S. Zhang, J. Hou, Adv. Mater. 2025, 37, 2418353.
- 33Z. Xia, C. Gao, Z. Xie, M. Wu, H. Chen, T. Li, J. Zhou, T. Cai, H. Hu, J. Shuai, C. Xie, G. Zhang, W. Chen, S. Liu, Angew. Chem. Int. Ed. 2025, 64, e202421953.
- 34Z. Li, Y. Xiang, J. Li, L. Feng, M. Zhang, Z. Zhang, S. Yan, B. Xu, Angew. Chem. Int. Ed. 2025, 64, e202413986.
- 35Z. Ge, J. Qiao, Y. Li, J. Song, X. Duan, Z. Fu, H. Hu, R. Yang, H. Yin, X. Hao, Y. Sun, Angew. Chem. Int. Ed. 2025, 64, e202413309.
- 36X. Song, L. Mei, X. Zhou, H. Li, H. Xu, X. Liu, S. Gao, S. Xu, Y. Yang, W. Zhu, J. Wang, X.-H. Zhang, X.-K. Chen, Angew. Chem. Int. Ed. 2024, 63, e202411512.
- 37T. Chen, Y. Zhong, T. Duan, X. Tang, W. Zhao, J. Wang, G. Lu, G. Long, J. Zhang, K. Han, X. Wan, B. Kan, Y. Chen, Angew. Chem. Int. Ed. 2025, 64, e202412983.
- 38C. Wang, Y. Xin, H. Gu, L. Ye, Y. Liu, Y. Zhou, Y. Deng, Y. Geng, Angew. Chem. Int. Ed. 2025, 64, e202415440.
- 39R. Yu, R. Shi, Z. He, T. Zhang, S. Li, Q. Lv, S. Sha, C. Yang, J. Hou, Z.'a. Tan, Angew. Chem. Int. Ed. 2023, 62, e202308367.
- 40P. Zhang, N. Gao, B. Du, Z. Xu, S. Wu, K. Zhu, X. Ma, H. Bin, Y. Li, Angew. Chem. Int. Ed. 2025, e202424430.
- 41Y. Wang, K. Sun, C. Li, C. Zhao, C. Gao, L. Zhu, Q. Bai, C. Xie, P. You, J. Lv, X. Sun, H. Hu, Z. Wang, H. Hu, Z. Tang, B. He, M. Qiu, S. Li, G. Zhang, Adv. Mater. 2024, 36, 2411957.
- 42J. Wang, Z. Zheng, Y. Ke, Y. Wang, X. Liu, L. Ye, S. Zhang, M. Zhang, J. Hou, Adv. Mater. 2025, 37, 2417160.
- 43S. Shoaee, H. M. Luong, J. Song, Y. Zou, T.-Q. Nguyen, D. Neher, Adv. Mater. 2024, 36, 2302005.
- 44C. Liu, L. Lüer, V. M. L. Corre, K. Forberich, P. Weitz, T. Heumüller, X. Du, J. Wortmann, J. Zhang, J. Wagner, L. Ying, J. Hauch, N. Li, C. J. Brabec, Adv. Mater. 2024, 36, 2300259.
- 45B. Sun, N. Tokmoldin, O. Alqahtani, A. Patterson, C. S. P. De Castro, D. B. Riley, M. Pranav, A. Armin, F. Laquai, B. A. Collins, D. Neher, S. Shoaee, Adv. Energy Mater. 2023, 13, 2300980.
- 46Y. Huang, Z. Yu, A. Yin, G.-F. Han, X.-Y. Lang, J.-L. Brédas, T. Wang, Q. Jiang, Angew. Chem. Int. Ed. 2025, 64, e202418225.
- 47X. Cao, P. Wang, X. Jia, W. Zhao, H. Chen, Z. Xiao, J. Li, X. Bi, Z. Yao, Y. Guo, G. Long, C. Li, X. Wan, Y. Chen, Angew. Chem. Int. Ed. 2025, 64, e202417244.
- 48X. Gu, Y. Wei, R. Zeng, J. Lv, Y. Hou, N. Yu, S. Tan, Z. Wang, C. Li, Z. Tang, Q. Peng, F. Liu, Y. Cai, X. Zhang, H. Huang, Angew. Chem. Int. Ed. 2025, 64, e202418926.
- 49K. Liu, Y. Jiang, G. Ran, F. Liu, W. Zhang, X. Zhu, Joule 2024, 8, 835–851.
- 50C. Li, J. Song, H. Lai, H. Zhang, R. Zhou, J. Xu, H. Huang, L. Liu, J. Gao, Y. Li, M. H. Jee, Z. Zheng, S. Liu, J. Yan, X.-K. Chen, Z. Tang, C. Zhang, H. Y. Woo, F. He, F. Gao, H. Yan, Y. Sun, Nat. Mater. 2025, 24, 433–443.
- 51S. Guan, Y. Li, C. Xu, N. Yin, C. Xu, C. Wang, M. Wang, Y. Xu, Q. Chen, D. Wang, L. Zuo, H. Chen, Adv. Mater. 2024, 36, 2400342.
- 52J. Zhou, L. Tan, Y. Liu, H. Li, X. Liu, M. Li, S. Wang, Y. Zhang, C. Jiang, R. Hua, W. Tress, S. Meloni, C. Yi, Joule 2024, 8, 1691–1706.
- 53D. He, F. Zhao, C. Wang, Y. Lin, Adv. Funct. Mater. 2022, 32, 2111855.
- 54Q. Liu, K. Vandewal, Adv. Mater. 2023, 35, 2302452.
- 55N. Zhang, T. Chen, Y. Li, S. Li, J. Yu, H. Liu, M. Wang, X.-K. Ye, X. Ding, X. Lu, C.-Z. Li, H. Zhu, M. Shi, H. Chen, Angew. Chem. Int. Ed. 2025, 64, e202420090.
- 56T. Duan, W. Feng, Y. Li, Z. Li, Z. Zhang, H. Liang, H. Chen, C. Zhong, S. Jeong, C. Yang, S. Chen, S. Lu, O. A. Rakitin, C. Li, X. Wan, B. Kan, Y. Chen, Angew. Chem. Int. Ed. 2023, 62, e202308832.
- 57B. Fan, W. Gao, R. Zhang, W. Kaminsky, L. Tang, F. R. Lin, Y. Wang, Q. Fan, W. Ma, F. Gao, A. K. Y. Jen, Angew. Chem. Int. Ed. 2023, 62, e202311559.
- 58Y. Lang, H. Lai, Y. Fu, R. Ma, P. W. K. Fong, H. Li, K. Liu, X. Yang, X. Lu, T. Yang, G. Li, F. He, Adv. Mater. 2025, 37, 2413270.
- 59K. Liu, Y. Jiang, F. Liu, G. Ran, F. Huang, W. Wang, W. Zhang, C. Zhang, J. Hou, X. Zhu, Adv. Mater. 2023, 35, 2300363.
- 60Y. Shi, L. Zhu, Y. Yan, M. Xie, G. Liang, J. Qiao, J. Zhang, X. Hao, K. Lu, Z. Wei, Adv. Energy Mater. 2023, 13, 2300458.
- 61L. Zhou, H. Yu, J. Zhang, D. Qiu, Y. Fu, J. Yi, L. Xie, X. Li, L. Meng, J. Zhang, X. Lu, Z. Wei, Y. Li, H. Yan, Angew. Chem. Int. Ed. 2024, 63, e202319635.
- 62T. Xu, Z. Luo, R. Ma, Z. Chen, T. A. Dela Peña, H. Liu, Q. Wei, M. Li, C.'e. Zhang, J. Wu, X. Lu, G. Li, C. Yang, Angew. Chem. Int. Ed. 2023, 62, e202304127.
- 63Z. Li, X. Li, J. Xue, J. Zhang, C. Zhu, J. Li, W. Ma, L. Meng, Y. Li, ACS Energy Lett. 2023, 8, 2488–2495.
- 64Y. Cho, Z. Sun, K. M. Lee, G. Zeng, S. Jeong, S. Yang, J. E. Lee, B. Lee, S.-H. Kang, Y. Li, Y. Li, S. K. Kwak, C. Yang, ACS Energy Lett. 2023, 8, 96–106.
- 65G. Chai, J. Zhang, M. Pan, Z. Wang, J. Yu, J. Liang, H. Yu, Y. Chen, A. Shang, X. Liu, F. Bai, R. Ma, Y. Chang, S. Luo, A. Zeng, H. Zhou, K. Chen, F. Gao, H. Ade, H. Yan, ACS Energy Lett. 2020, 5, 3415–3425.
- 66C. Yang, Q. An, M. Jiang, X. Ma, A. Mahmood, H. Zhang, X. Zhao, H.-F. Zhi, M. H. Jee, H. Y. Woo, X. Liao, D. Deng, Z. Wei, J.-L. Wang, Angew. Chem. Int. Ed. 2023, 62, e202313016.
- 67X. Zhao, Q. An, H. Zhang, C. Yang, A. Mahmood, M. Jiang, M. H. Jee, B. Fu, S. Tian, H. Y. Woo, Y. Wang, J.-L. Wang, Angew. Chem. Int. Ed. 2023, 62, e202216340.
- 68J. Zhang, S. Luo, H. Zhao, X. Xu, X. Zou, A. Shang, J. Liang, F. Bai, Y. Chen, K. S. Wong, Z. Ma, W. Ma, H. Hu, Y. Chen, H. Yan, Angew. Chem. Int. Ed. 2022, 61, e202206930.
- 69B. Fan, W. Gao, R. Zhang, W. Kaminsky, F. R. Lin, X. Xia, Q. Fan, Y. Li, Y. An, Y. Wu, M. Liu, X. Lu, W. J. Li, H.-L. Yip, F. Gao, A. K. Y. Jen, J. Am. Chem. Soc. 2023, 145, 5909–5919.
- 70J. Fu, Q. Yang, P. Huang, S. Chung, K. Cho, Z. Kan, H. Liu, X. Lu, Y. Lang, H. Lai, F. He, P. W. K. Fong, S. Lu, Y. Yang, Z. Xiao, G. Li, Nat. Commun. 2024, 15, 1830.
- 71Z. Chen, J. Zhu, D. Yang, W. Song, J. Shi, J. Ge, Y. Guo, X. Tong, F. Chen, Z. Ge, Energy Environ. Sci. 2023, 16, 3119–3127.
- 72X. Kong, C. Zhu, J. Zhang, L. Meng, S. Qin, J. Zhang, J. Li, Z. Wei, Y. Li, Energy Environ. Sci. 2022, 15, 2011–2020.
- 73Q. Yang, H. Chen, J. Lv, P. Huang, D. Han, W. Deng, K. Sun, M. Kumar, S. Chung, K. Cho, D. Hu, H. Dong, L. Shao, F. Zhao, Z. Xiao, Z. Kan, S. Lu, Adv. Sci. 2023, 10, 2207678.
- 74J. Shi, Z. Chen, H. Liu, Y. Qiu, S. Yang, W. Song, Z. Ge, Adv. Energy Mater. 2023, 13, 2301292.
- 75Y. Zhang, Y. Ji, Y. Zhang, W. Zhang, H. Bai, M. Du, H. Wu, Q. Guo, E. Zhou, Adv. Funct. Mater. 2022, 32, 2205115.
- 76S. Chen, S. Zhu, L. Hong, W. Deng, Y. Zhang, Y. Fu, Z. Zhong, M. Dong, C. Liu, X. Lu, K. Zhang, F. Huang, Angew. Chem. Int. Ed. 2024, 63, e202318756.
- 77H. Yin, Y. Cui, D. Chen, S. Liu, T. Wu, M. Yu, L. Ye, A. Liang, Y. Chen, J. Am. Chem. Soc. 2025, 147, 8796–8808.
- 78J. Wang, Y. Cui, Z. Chen, J. Zhang, Y. Xiao, T. Zhang, W. Wang, Y. Xu, N. Yang, H. Yao, X.-T. Hao, Z. Wei, J. Hou, J. Am. Chem. Soc. 2023, 145, 13686–13695.
- 79Z. Luo, T. Liu, J. Oh, R. Ma, J. Miao, F. Ni, G. Zhang, R. Sun, C.'e. Zhang, Z. Chen, Y. Zou, J. Min, C. Yang, H. Yan, C. Yang, Adv. Funct. Mater. 2022, 32, 2203200.
- 80F. Meng, Y. Qin, Y. Zheng, Z. Zhao, Y. Sun, Y. Yang, K. Gao, D. Zhao, Angew. Chem. Int. Ed. 2023, 62, e202217173.
- 81W. Liu, S. Sun, L. Zhou, Y. Cui, W. Zhang, J. Hou, F. Liu, S. Xu, X. Zhu, Angew. Chem. Int. Ed. 2022, 61, e202116111.
- 82W. Gao, H. Fu, Y. Li, F. Lin, R. Sun, Z. Wu, X. Wu, C. Zhong, J. Min, J. Luo, H. Y. Woo, Z. Zhu, A. K. Y. Jen, Adv. Energy Mater. 2021, 11, 2003177.
- 83H. Hu, S. Liu, J. Xu, R. Ma, Z. Peng, T. A. D. Peña, Y. Cui, W. Liang, X. Zhou, S. Luo, H. Yu, M. Li, J. Wu, S. Chen, G. Li, Y. Chen, Angew. Chem. Int. Ed. 2024, 63, e202400086.
- 84H. Chen, Y. Huang, R. Zhang, H. Mou, J. Ding, J. Zhou, Z. Wang, H. Li, W. Chen, J. Zhu, Q. Cheng, H. Gu, X. Wu, T. Zhang, Y. Wang, H. Zhu, Z. Xie, F. Gao, Y. Li, Y. Li, Nat. Mater. 2025, 24, 444–453.
- 85J. Guo, S. Qin, J. Zhang, C. Zhu, X. Xia, Y. Gong, T. Liang, Y. Zeng, G. Han, H. Zhuo, Y. Li, L. Meng, Y. Yi, J. Chen, X. Li, B. Qiu, Y. Li, Nat. Commun. 2025, 16, 1503.
- 86H. Gao, Q. Li, B. Fan, Z. Bi, W. Jiang, S. Zhang, Q. Fan, T. Chen, F. R. Lin, B. Kan, D. Lei, W. Ma, A. K. Y. Jen, Adv. Energy Mater. 2024, 2403121.
- 87J. Hai, Y. Song, L. Li, X. Liu, X. Shi, Z. Huang, G. Qian, Z. Lu, J. Yu, H. Hu, S. Chen, Adv. Funct. Mater. 2023, 33, 2213429.
- 88Y. Chen, Z. Wu, L. Ding, S. Zhang, Z. Chen, W. Li, Y. Zhao, Y. Wang, Y. Liu, Adv. Funct. Mater. 2023, 33, 2304316.
- 89C. Xiao, X. Wang, T. Zhong, R. Zhou, X. Zheng, Y. Liu, T. Hu, Y. Luo, F. Sun, B. Xiao, Z. Liu, C. Yang, R. Yang, Adv. Sci. 2023, 10, 2206580.
- 90Z. Luo, Y. Gao, H. Lai, Y. Li, Z. Wu, Z. Chen, R. Sun, J. Ren, C.'e. Zhang, F. He, H. Woo, J. Min, C. Yang, Energy Environ. Sci. 2022, 15, 4601–4611.
- 91Y. Chen, R. Ma, T. Liu, Y. Xiao, H. K. Kim, J. Zhang, C. Ma, H. Sun, F. Bai, X. Guo, K. S. Wong, X. Lu, H. Yan, Adv. Energy Mater. 2021, 11, 2003777.
- 92B. Zou, A. Liang, P. Ding, J. Yao, X. Zeng, H. Li, R. Ma, C. Li, W. Wu, D. Chen, M. Qammar, H. Yu, J. Yi, L. Guo, S. H. Pun, J. E. Halpert, G. Li, Z. Kan, H. Yan, Angew. Chem. Int. Ed. 2025, 64, e202415332.
- 93H. Yang, S. Bao, N. Cui, H. Fan, K. Hu, C. Cui, Y. Li, Angew. Chem. Int. Ed. 2023, 62, e202216338.
- 94Y. Cui, P. Zhu, H. Hu, X. Xia, X. Lu, S. Yu, H. Tempeld, R.-A. Eichel, X. Liao, Y. Chen, Angew. Chem. Int. Ed. 2023, 62, e202304931.
- 95T. Chen, S. Li, Y. Li, Z. Chen, H. Wu, Y. Lin, Y. Gao, M. Wang, G. Ding, J. Min, Z. Ma, H. Zhu, L. Zuo, H. Chen, Adv. Mater. 2023, 35, 2300400.
- 96X. Liu, Y. Zhao, Y. Ni, F. Shi, X. Guo, C. Li, Energy Environ. Sci. 2023, 16, 4065–4072.
- 97Y. Jiang, S. Sun, R. Xu, F. Liu, X. Miao, G. Ran, K. Liu, Y. Yi, W. Zhang, X. Zhu, Nat. Energy 2024, 9, 975–986.
- 98L. Yan, H. Zhang, Q. An, M. Jiang, A. Mahmood, M.H. Jee, H.-R. Bai, H.-F. Zhi, S. Zhang, H. Y. Woo, J.-L. Wang, Angew. Chem. Int. Ed. 2022, 61, e202209454.
- 99Q. Fan, R. Ma, J. Yang, J. Gao, H. Bai, W. Su, Z. Liang, Y. Wu, L. Tang, Y. Li, Q. Wu, K. Wang, L. Yan, R. Zhang, F. Gao, G. Li, W. Ma, Angew. Chem. Int. Ed. 2023, 62, e202308307.
- 100L. Xie, A. Lan, Q. Gu, S. Yang, W. Song, J. Ge, R. Zhou, Z. Chen, J. Zhang, X. Zhang, D. Yang, B. Tang, T. Wu, Z. Ge, ACS Energy Lett. 2023, 8, 361–371.
- 101Z. Li, X. Kong, Z. Chen, I. Angunawela, H. Zhu, X. Li, L. Meng, H. Ade, Y. Li, ACS Appl. Mater. Inter. 2022, 14, 52058–52066.
- 102R. Xu, Y. Jiang, F. Liu, W. Su, W. Liu, S. Xu, H. Fan, C. Jiang, Q. Zong, W. Zhang, X. Zhu, Chem. Eng. J. 2023, 464, 142507.
- 103Y. Zhou, G. Qi, H. Liu, H. Bai, T. Li, M. H. Maqsood, C. Liu, B. Song, N. Chen, G. Lu, C. Gao, Y. Liu, W. Su, H. Du, R. Ma, W. Ma, Q. Fan, Sci. China Mater. 2024, 68, 850–859.
- 104Z. Chen, Y. Xiao, H. Yao, J. Ren, T. Zhang, J. Qiao, S. Zhu, R. Lin, X. Hao, J. Hou, Adv. Mater. 2024, 36, 2408858.
- 105X. Li, R. Peng, Y. Qiu, Y. Zhang, J. Shi, S. Gao, H. Liu, F. Jin, Z. Ge, Adv. Funct. Mater. 2025, 35, 2413259.
- 106W. Feng, Y. Bai, J. Wang, Y. Zhong, J. Wang, T. Chen, J. Zhang, K. Han, X. Wan, B. Kan, Y. Chen, Adv. Energy Mater. 2024, 14, 2404062.
- 107J. Shi, P. Ding, J. Zhu, Z. Chen, S. Gao, X. Yu, X. Liao, Q. Liu, Z. Ge, Energy Environ. Sci. 2024, 17, 9144–9153.
- 108Z. Zhang, Y. Li, G. Cai, Y. Zhang, X. Lu, Y. Lin, J. Am. Chem. Soc. 2020, 142, 18741–18745.
- 109W. Gao, R. Ma, L. Zhu, L. Li, F. R. Lin, T. A. Dela Peña, J. Wu, M. Li, W. Zhong, X. Wu, Z. Fink, C. Tian, F. Liu, Z. Wei, A. K. Y. Jen, Li G., Adv. Energy Mater. 2024, 14, 2304477.
- 110F. Qi, L. O. Jones, K. Jiang, S.-H. Jang, W. Kaminsky, J. Oh, H. Zhang, Z. Cai, C. Yang, K. L. Kohlstedt, G. C. Schatz, F. R. Lin, T. J. Marks, Jen A. K. Y., Mater. Horiz. 2022, 9, 403–410.
- 111Z. Jia, Q. Ma, Z. Chen, L. Meng, N. Jain, I. Angunawela, S. Qin, X. Kong, X. Li, Y. Yang, H. Zhu, H. Ade, F. Gao, Y. Li, Nat. Commun. 2023, 14, 1236.
- 112F. Huang, Z. Li, G. Song, C. Jiang, Y. Yang, J. Wang, X. Wan, C. Li, Z. Yao, Y. Chen, Adv. Funct. Mater. 2023, 33, 2211140.
- 113K. Jiang, J. Zhang, C. Zhong, F. R. Lin, F. Qi, Q. Li, Z. Peng, W. Kaminsky, S.-H. Jang, J. Yu, X. Deng, H. Hu, D. Shen, F. Gao, H. Ade, M. Xiao, C. Zhang, A. K. Y. Jen, Nat. Energy 2022, 7, 1076–1086.
- 114J. Tao, K. Yang, D. Qiu, C. Wang, H. Zhang, M. Lv, J. Zhang, K. Lu, Z. Wei, Nano Energy 2024, 125, 109540.
- 115L. Li, W. Gao, R. Ma, X. Zhao, T. A. Dela Peña, J. Wu, J.-X. Tang, Z. Wei, Sci. China Chem. 2024, https://doi.org/10.1007/s11426-024-2381-0
- 116K.-H. Huang, C.-C. Tseng, C.-L. Tsai, Y.-J. Xue, H.-C. Lu, C.-F. Lu, Y.-Y. Chang, C.-L. Huang, I. J. Hsu, Y.-Y. Lai, Y.-P. Zheng, B.-H. Jiang, C.-P. Chen, S.-Y. Chien, U. S. Jeng, C.-S. Hsu, Y.-J. Cheng, Adv. Funct. Mater. 2024, 35, 2419176.
- 117C. Tang, X. Ma, J.-Y. Wang, X. Zhang, R. Liao, Y. Ma, P. Wang, P. Wang, T. Wang, F. Zhang, Q. Zheng, Angew. Chem. Int. Ed. 2021, 60, 19314–19323.
- 118C. Yang, Q. An, H.-R. Bai, H.-F. Zhi, H. S. Ryu, A. Mahmood, X. Zhao, S. Zhang, H. Y. Woo, J.-L. Wang, Angew. Chem. Int. Ed. 2021, 60, 19241–19252.
- 119W. Gao, F. Qi, Z. Peng, F. R. Lin, K. Jiang, C. Zhong, W. Kaminsky, Z. Guan, C.-S. Lee, T. J. Marks, H. Ade, A. K. Y. Jen, Adv. Mater. 2022, 34, 2202089.
- 120Y. Gao, X. Yang, W. Wang, R. Sun, J. Cui, Y. Fu, K. Li, M. Zhang, C. Liu, H. Zhu, X. Lu, J. Min, Adv. Mater. 2023, 35, 2300531.
- 121Z. Chen, S. Zhang, T. Zhang, J. Ren, J. Dai, H. Li, J. Qiao, X. Hao, J. Hou, Angew. Chem. Int. Ed. 2024, 63, e202317892.
- 122C. He, Y. Pan, Y. Ouyang, Q. Shen, Y. Gao, K. Yan, J. Fang, Y. Chen, C.-Q. Ma, J. Min, C. Zhang, L. Zuo, H. Chen, Energy Environ. Sci. 2022, 15, 2537–2544.
- 123X. Li, I. Angunawela, Y. Chang, J. Zhou, H. Huang, L. Zhong, A. Liebman-Pelaez, C. Zhu, L. Meng, Z. Xie, H. Ade, H. Yan, Y. Li, Energy Environ. Sci. 2020, 13, 5028–5038.
- 124Y. Xu, H. Yao, L. Ma, L. Hong, J. Li, Q. Liao, Y. Zu, J. Wang, M. Gao, L. Ye, J. Hou, Angew. Chem. Int. Ed. 2020, 59, 9004–9010.
- 125G. Li, L.-W. Feng, S. Mukherjee, L. O. Jones, R. M. Jacobberger, W. Huang, R. M. Young, R. M. Pankow, W. Zhu, N. Lu, K. L. Kohlstedt, V. K. Sangwan, M. R. Wasielewski, M. C. Hersam, G. C. Schatz, D. M. DeLongchamp, A. Facchetti, T. J. Marks, Energy Environ. Sci. 2022, 15, 645–659.
- 126Y. Cui, H. Yao, J. Zhang, T. Zhang, Y. Wang, L. Hong, K. Xian, B. Xu, S. Zhang, J. Peng, Z. Wei, F. Gao, J. Hou, Nat. Commun. 2019, 10, 2515.
- 127H. Shi, H. Guo, D. Cai, J.-Y. Wang, Y. Ma, Q. Zheng, Energy Environ. Sci. 2025, 18, 2895–2904.
- 128H. Lai, Y. Lang, Y. Luo, Z. Deng, Y. Wang, D. Qiu, R. Sun, G. Zhang, J. Wu, G. Li, F. He, Adv. Energy Mater. 2025, 15, 2406097.
- 129N. Niharika Bhuyan, S. Shankar S, S. Jyoti Panda, C. Shekhar Purohit, R. Singhal, G. D. Sharma, A. Mishra, Angew. Chem. Int. Ed. 2024, 63, e202406272.
- 130T. Dai, A. Tang, Y. Meng, C. Dong, P. Cong, J. Lu, J. Du, Y. Zhong, E. Zhou, Angew. Chem. Int. Ed. 2024, 63, e202403051.
- 131 Deposition numbers 2362915 (for DASe-4Cl) and 2362914 (for TASe-2F2Cl) contain the supplementary crystallographic data for this paper. These data are provided free of charge by the joint Cambridge Crystallographic Data Centre.
- 132J. Wu, G. Li, J. Fang, X. Guo, L. Zhu, B. Guo, Y. Wang, G. Zhang, L. Arunagiri, F. Liu, H. Yan, M. Zhang, Y. Li, Nat. Commun. 2020, 11, 4612.
- 133Y. Xie, C. Zhou, X. Ma, S. Y. Jeong, H. Y. Woo, F. Huang, Y. Yang, H. Yu, J. Li, F. Zhang, K. Wang, X. Zhu, Adv. Energy Mater. 2024, 14, 2400013.
- 134K. Zhou, K. Xian, R. Ma, J. Liu, M. Gao, S. Li, T. Liu, Y. Chen, Y. Geng, L. Ye, Energy Environ. Sci. 2023, 16, 5052–5064.
- 135J. S. Park, G.-U. Kim, S. Lee, J.-W. Lee, S. Li, J.-Y. Lee, B. J. Kim, Adv. Mater. 2022, 34, 2201623.
- 136H.-R. Bai, H. Zhang, H. Meng, Y. Li, X. Xu, M.-Q. Liu, Y. Chen, Z. F. Yao, H. F. Zhi, A. Mahmood, Y. Wang, J. Ye, M. Jiang, Q. An, H. Y. Woo, H. Wu, Q. Peng, J.-L. Wang, Mater. SCi.Eng. R. Rep. 2025, 163, 100916.
