Key Takeaways & Executive Findings
- •• • PTzEH-F achieves 19.17% PCE as-cast from toluene without additives or post-treatments, demonstrating a viable route to eco-friendly processing while maintaining high efficiency. • • The ternary LbL device (PTzEH-F/L8-BO:PC71BM) reaches 20.27% PCE, indicating that DTzBT-based donors can be integrated into advanced device architectures for further gains. • • PTzMe-F, with N-methyl side chains, yields only 2.64% PCE (chloroform) due to poor solubility and miscibility with L8-BO, underscoring the critical role of side-chain engineering in morphology control. • • DTzBT building block lowers HOMO levels via thiazole fusion, enabling higher VOC while maintaining aggregation tunability, as evidenced by the improved performance of PTzEH-F over PTzMe-F.
Abstract
Developing organic solar cells (OSCs) processable from green solvents without additives or post-treatments is essential for sustainable manufacturing, yet high power conversion efficiency (PCE) remains difficult due to limited morphology control. Herein, we develop a new electron-deficient building block, dithiazolo[4',5':3,4;5'',4'':5,6]benzo[1,2-d][1,2,3]triazole (DTzBT), which fuses benzo[d][1,2,3]triazole (BTA) with thiazole to leverage S/N-mediated non-covalent interactions, enhance planarity and lower the HOMO. To isolate side-chain effects, two DTzBT-based donors, namely PTzMe-F (N-methyl) and PTzEH-F (N-2-ethylhexyl), have been designed and synthesized. PTzMe-F exhibits poor solubility and miscibility with L8-BO, yielding 2.64% PCE (chloroform). PTzEH-F exhibits excellent processability and favorable morphology, delivering 17.61% PCE (chloroform) and 19.17% as-cast from toluene without any additive or post-treatments. In addition, the ternary LbL device based on PTzEH-F/L8-BO:PC71BM achieved an impressive efficiency of 20.27%. Comprehensive characterization indicates that 2-ethylhexyl side chains afford optimal solubility while preserving strong intermolecular interactions and favorable phase separation. DTzBT mitigates BTA’s HOMO-raising tendency via electron-withdrawing thiazole fusion, reconciling aggregation tunability with energy-level control. These results show that precise backbone and side-chain co-design enables green-solvent, additive-free processing for high-performance OSCs, advancing sustainable photovoltaic manufacturing.
1. Introduction
Organic solar cells (OSCs) have achieved power conversion efficiencies exceeding 20% through advances in non-fullerene acceptors and polymer donor design. However, scalable manufacturing is hindered by reliance on halogenated solvents, processing additives, and post-treatments, which raise environmental and economic costs. Achieving high efficiency under green-solvent, additive-free, as-cast conditions is a critical bottleneck for industrial adoption.
This work addresses that bottleneck by introducing a novel electron-deficient building block, dithiazolobenzotriazole (DTzBT), which fuses benzotriazole with thiazole to enhance planarity and lower HOMO levels. By systematically varying side chains (methyl vs. 2-ethylhexyl), the authors demonstrate that side-chain engineering is key to balancing solubility, intermolecular interactions, and phase separation, enabling efficient as-cast devices from toluene. This co-design strategy offers a practical pathway to sustainable OSCs without compromising performance.
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Huoqing Yang, Chentong Liao, Xingjian Dai, Weilin Zhou, Yihui Wu, Xiaopeng Xu, Qiang Peng (2026). Efficient green-solvent, additive-free and post-treatment-free organic solar cells enabled by dithiazolobenzotriazole-based polymer donors. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-026-4246-5
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Frequently Asked Questions
What is the impact of side-chain choice on the photovoltaic performance of DTzBT-based donors?
The N-methyl side chain (PTzMe-F) results in poor solubility and miscibility with L8-BO, yielding only 2.64% PCE in chloroform. In contrast, the N-2-ethylhexyl side chain (PTzEH-F) provides optimal solubility and favorable morphology, achieving 17.61% PCE in chloroform and 19.17% as-cast from toluene. This demonstrates that side-chain engineering is critical for balancing processability and performance.
How does the DTzBT building block improve energy levels compared to conventional BTA?
DTzBT fuses thiazole to BTA, leveraging S/N-mediated non-covalent interactions to enhance planarity and lower the HOMO level. This mitigates BTA's tendency to raise HOMO, allowing for higher open-circuit voltage (VOC) while maintaining aggregation tunability, as evidenced by the improved performance of PTzEH-F.
What are the efficiency benchmarks for green-solvent processed OSCs in this study?
PTzEH-F achieves 19.17% PCE as-cast from toluene without any additive or post-treatment. In a ternary layer-by-layer (LbL) device with L8-BO:PC71BM, the efficiency reaches 20.27%, setting a high benchmark for sustainable processing.
What is the significance of the ternary LbL device architecture in this work?
The ternary LbL device (PTzEH-F/L8-BO:PC71BM) achieves 20.27% PCE, demonstrating that DTzBT-based donors can be effectively integrated into more complex device architectures to further enhance performance, potentially by improving light absorption and charge transport.
What are the implications of this work for industrial manufacturing of OSCs?
By demonstrating high efficiency (19.17%) using toluene as a green solvent and eliminating additives and post-treatments, this work reduces environmental and economic costs, making roll-to-roll manufacturing more feasible. The co-design of backbone and side chains offers a strategy for developing processable, high-performance materials.
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