| 1. |
- Feng, Kui, et al.
(author)
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Fused Bithiophene Imide Dimer-Based n-Type Polymers for High-Performance Organic Electrochemical Transistors
- 2021
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In: Angewandte Chemie International Edition. - : WILEY-V C H VERLAG GMBH. - 1433-7851 .- 1521-3773. ; 60:45, s. 24198-24205
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Journal article (peer-reviewed)abstract
- The development of n-type organic electrochemical transistors (OECTs) lags far behind their p-type counterparts. In order to address this dilemma, we report here two new fused bithiophene imide dimer (f-BTI2)-based n-type polymers with a branched methyl end-capped glycol side chain, which exhibit good solubility, low-lying LUMO energy levels, favorable polymer chain orientation, and efficient ion transport property, thus yielding a remarkable OECT electron mobility (mu(e)) of up to approximate to 10(-2) cm(2) V-1 s(-1) and volumetric capacitance (C*) as high as 443 F cm(-3), simultaneously. As a result, the f-BTI2TEG-FT-based OECTs deliver a record-high maximum geometry-normalized transconductance of 4.60 S cm(-1) and a maximum mu C* product of 15.2 F cm(-1) V-1 s(-1). The mu C* figure of merit is more than one order of magnitude higher than that of the state-of-the-art n-type OECTs. The emergence of f-BTI2TEG-FT brings a new paradigm for developing high-performance n-type polymers for low-power OECT applications.
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| 2. |
- Guo, Han, et al.
(author)
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Transition metal-catalysed molecular n-doping of organic semiconductors
- 2021
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In: Nature. - London, United Kingdom : Nature Publishing Group. - 0028-0836 .- 1476-4687. ; 599:7883, s. 67-73
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Journal article (peer-reviewed)abstract
- Electron doping of organic semiconductors is typically inefficient, but here a precursor molecular dopant is used to deliver higher n-doping efficiency in a much shorter doping time. Chemical doping is a key process for investigating charge transport in organic semiconductors and improving certain (opto)electronic devices(1-9). N(electron)-doping is fundamentally more challenging than p(hole)-doping and typically achieves a very low doping efficiency (eta) of less than 10%(1,10). An efficient molecular n-dopant should simultaneously exhibit a high reducing power and air stability for broad applicability(1,5,6,9,11), which is very challenging. Here we show a general concept of catalysed n-doping of organic semiconductors using air-stable precursor-type molecular dopants. Incorporation of a transition metal (for example, Pt, Au, Pd) as vapour-deposited nanoparticles or solution-processable organometallic complexes (for example, Pd-2(dba)(3)) catalyses the reaction, as assessed by experimental and theoretical evidence, enabling greatly increased eta in a much shorter doping time and high electrical conductivities (above 100 S cm(-1); ref. (12)). This methodology has technological implications for realizing improved semiconductor devices and offers a broad exploration space of ternary systems comprising catalysts, molecular dopants and semiconductors, thus opening new opportunities in n-doping research and applications(12, 13).
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| 3. |
- Tang, Yumin, et al.
(author)
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Two Compatible Polymer Donors Enabling Ternary Organic Solar Cells with a Small Nonradiative Energy Loss and Broad Composition Tolerance
- 2020
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In: Solar RRL. - : Wiley-VCH Verlagsgesellschaft. - 2367-198X. ; 4:11
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Journal article (peer-reviewed)abstract
- High-performance nonfullerene ternary organic solar cells (OSCs) with two polymer donors are less frequently reported because of the limited numbers of efficient polymer donors with good compatibility. Herein, a wide-bandgap polymer P1 with a deep-lying highest occupied molecular orbital (HOMO) level is incorporated as the third component into the benchmark PM6:Y6 binary system to fabricate ternary OSCs. The introduction of P1 not only leads to extended absorption coverage and forms a cascade-like energy level alignment but also shows excellent compatibility with PM6, resulting in a favorable morphology in the ternary blend. More importantly, P1 possesses a deeper HOMO level (-5.6 eV) than most well-known donor polymers, which enables resulting ternary OSCs with an improved open-circuit voltage. As a result, the optimized ternary OSCs with 40 wt% P1 in donors achieve a power conversion efficiency (PCE) of 16.2% with a small nonradiative recombination loss of 0.23 eV, which is among the highest values of ternary OSCs based on two polymer donors. In addition, the ternary OSCs show a broad composition tolerance with a high PCE of over 14% throughout the whole blend ratios. These results provide an effective approach to fabricate efficient ternary OSCs by synergizing two wide-bandgap polymer donors.
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| 4. |
- Chen, Jianhua, et al.
(author)
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Highly stretchable organic electrochemical transistors with strain-resistant performance
- 2022
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In: Nature Materials. - : NATURE PORTFOLIO. - 1476-1122 .- 1476-4660. ; 21, s. 564-571
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Journal article (peer-reviewed)abstract
- Realizing fully stretchable electronic materials is central to advancing new types of mechanically agile and skin-integrable optoelectronic device technologies. Here we demonstrate a materials design concept combining an organic semiconductor film with a honeycomb porous structure with biaxially prestretched platform that enables high-performance organic electrochemical transistors with a charge transport stability over 30-140% tensional strain, limited only by metal contact fatigue. The prestretched honeycomb semiconductor channel of donor-acceptor polymer poly(2,5-bis(2-octyldodecyl)-3,6-di(thiophen-2-yl)-2,5-diketo-pyrrolopyrrole-alt-2,5-bis(3-triethyleneglycoloxy-thiophen-2-yl) exhibits high ion uptake and completely stable electrochemical and mechanical properties over 1,500 redox cycles with 10(4) stretching cycles under 30% strain. Invariant electrocardiogram recording cycles and synapse responses under varying strains, along with mechanical finite element analysis, underscore that the present stretchable organic electrochemical transistor design strategy is suitable for diverse applications requiring stable signal output under deformation with low power dissipation and mechanical robustness. Highly stretchable organic electrochemical transistors with stable charge transport under severe tensional strains are demonstrated using a honeycomb semiconducting polymer morphology, thereby enabling controllable signal output for diverse stretchable bioelectronic applications.
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| 5. |
- Liu, Tao, et al.
(author)
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16% efficiency all-polymer organic solar cells enabled by a finely tuned morphology via the design of ternary blend
- 2021
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In: Joule. - : CELL PRESS. - 2542-4351. ; 5:4, s. 914-930
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Journal article (peer-reviewed)abstract
- A SUMMARY There is an urgent demand for all-polymer organic solar cells (AP-OSCs) to gain higher efficiency. Here, we successfully improve the performance to 16.09% by introducing a small amount of BN-T, a B <- N-type polymer acceptor, into the PM6:PY-IT blend. It has been found that BN-T makes the active layer, based on the PM6:PY-IT:BN-T ternary blend, more crystalline but meanwhile slightly reduces the phase separation, leading to enhancement of both exciton harvesting and charge transport. From a thermodynamic viewpoint, BN-T prefers to reside between PM6 and PY-IT, and the fraction of this fine-tunes the morphology. Besides, a significantly reduced nonradiative energy loss occurs in the ternary blend, along with the coexistence of energy and charge transfer between the two acceptors. The progressive performance facilitated by these improved properties demonstrates that AP-OSCs can possibly comparably efficient with those based on small molecule acceptors, further enhancing the competitiveness of this device type.
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| 6. |
- Shi, Yongqiang, et al.
(author)
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Thiazole Imide-Based All-Acceptor Homopolymer with Branched Ethylene Glycol Side Chains for Organic Thermoelectrics
- 2022
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In: Angewandte Chemie International Edition. - : WILEY-V C H VERLAG GMBH. - 1433-7851 .- 1521-3773. ; 61:51
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Journal article (peer-reviewed)abstract
- n-Type semiconducting polymers with high thermoelectric performance remain challenging due to the scarcity of molecular design strategy, limiting their applications in organic thermoelectric (OTE) devices. Herein, we provide a new approach to enhance the OTE performance of n-doped polymers by introducing acceptor-acceptor (A-A) type backbone bearing branched ethylene glycol (EG) side chains. When doped with 4-(2,3-dihydro-1,3-dimethyl-1H-benzimidazol-2-yl)-N,N-dimethylbenzenamine (N-DMBI), the A-A homopolymer PDTzTI-TEG exhibits n-type electrical conductivity (sigma) up to 34 S cm(-1) and power factor value of 15.7 mu W m(-1) K-2. The OTE performance of PDTzTI-TEG is far greater than that of homopolymer PBTI-TEG (sigma=0.27 S cm(-1)), indicating that introducing electron-deficient thiazole units in the backbone further improves the n-doping efficiency. These results demonstrate that developing A-A type polymers with EG side chains is an effective strategy to enhance n-type OTE performance.
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| 7. |
- Sun, Huiliang, et al.
(author)
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A monothiophene unit incorporating both fluoro and ester substitution enabling high-performance donor polymers for non-fullerene solar cells with 16.4% efficiency
- 2019
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In: Energy & Environmental Science. - : ROYAL SOC CHEMISTRY. - 1754-5692 .- 1754-5706. ; 12:11, s. 3328-3337
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Journal article (peer-reviewed)abstract
- Thiophene and its derivatives have been extensively used in organic electronics, particularly in the field of polymer solar cells (PSCs). Significant research efforts have been dedicated to modifying thiophene-based units by attaching electron-donating or withdrawing groups to tune the energy levels of conjugated materials. Herein, we report the design and synthesis of a novel thiophene derivative, FE-T, featuring a monothiophene functionalized with both an electron-withdrawing fluorine atom (F) and an ester group (E). The FE-T unit possesses distinctive advantages of both F and E groups, the synergistic effects of which enable significant downshifting of the energy levels and enhanced aggregation/crystallinity of the resulting organic materials. Shown in this work are a series of polymers obtained by incorporating the FE-T unit into a PM6 polymer to fine-tune the energetics and morphology of this high-performance PSC material. The optimal polymer in the series shows a downshifted HOMO and an improved morphology, leading to a high PCE of 16.4% with a small energy loss (0.53 eV) enabled by the reduced non-radiative energy loss (0.23 eV), which are among the best values reported for non-fullerene PSCs to date. This work shows that the FE-T unit is a promising building block to construct donor polymers for high-performance organic photovoltaic cells.
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| 8. |
- Sun, Huiliang, et al.
(author)
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A Narrow-Bandgap n-Type Polymer with an Acceptor-Acceptor Backbone Enabling Efficient All-Polymer Solar Cells
- 2020
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In: Advanced Materials. - : WILEY-V C H VERLAG GMBH. - 0935-9648 .- 1521-4095. ; 32
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Journal article (peer-reviewed)abstract
- Narrow-bandgap polymer semiconductors are essential for advancing the development of organic solar cells. Here, a new narrow-bandgap polymer acceptor L14, featuring an acceptor-acceptor (A-A) type backbone, is synthesized by copolymerizing a dibrominated fused-ring electron acceptor (FREA) with distannylated bithiophene imide. Combining the advantages of both the FREA and the A-A polymer, L14 not only shows a narrow bandgap and high absorption coefficient, but also low-lying frontier molecular orbital (FMO) levels. Such FMO levels yield improved electron transfer character, but unexpectedly, without sacrificing open-circuit voltage (V-oc), which is attributed to a small nonradiative recombination loss (E-loss,E-nr) of 0.22 eV. Benefiting from the improved photocurrent along with the high fill factor andV(oc), an excellent efficiency of 14.3% is achieved, which is among the highest values for all-polymer solar cells (all-PSCs). The results demonstrate the superiority of narrow-bandgap A-A type polymers for improving all-PSC performance and pave a way toward developing high-performance polymer acceptors for all-PSCs.
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| 9. |
- Sun, Huiliang, et al.
(author)
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Reducing energy loss via tuning energy levels of polymer acceptors for efficient all-polymer solar cells
- 2020
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In: Science China Chemistry. - : Springer Science and Business Media LLC. - 1869-1870 .- 1674-7291. ; 63:12, s. 1785-1792
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Journal article (peer-reviewed)abstract
- The open-circuit voltage (Voc) of all-polymer solar cells (all-PSCs) is typically lower than 0.9 V even for the most efficient ones. Large energy loss is the main reason for limiting Voc and efficiency of all-PSCs. Herein, through materials design using electron deficient building blocks based on bithiophene imides, the lowest unoccupied molecular orbital (LUMO) energy levels of polymer acceptors can be effectively tuned, which resulted in a reduced energy loss induced by charge generation and recombination loss due to the suppressed charge-transfer (CT) state absorption. Despite a negligible driving force, all-PSC based on the polymer donor and acceptor combination with well-aligned energy levels exhibited efficient charge transfer and achieved an external quantum efficiency over 10% while maintaining a large Voc of 1.02 V, leading to a 9.21% efficiency. Through various spectroscopy approaches, this work sheds light on the mechanism of energy loss in all-PSCs, which paves an avenue to achieving efficient all-PSCs with large Voc and drives the further development of all-PSCs.
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| 10. |
- Sun, Huiliang, et al.
(author)
-
Reducing energy lossviatuning energy levels of polymer acceptors for efficient all-polymer solar cells
- 2020
-
In: Science China Chemistry. - : Science China Press and Springer-Verlag GmbH Germany. - 1674-7291 .- 1869-1870. ; 63, s. 1785-1792
-
Journal article (peer-reviewed)abstract
- The open-circuit voltage (V-oc) of all-polymer solar cells (all-PSCs) is typically lower than 0.9 V even for the most efficient ones. Large energy loss is the main reason for limitingV(oc)and efficiency of all-PSCs. Herein, through materials design using electron deficient building blocks based on bithiophene imides, the lowest unoccupied molecular orbital (LUMO) energy levels of polymer acceptors can be effectively tuned, which resulted in a reduced energy loss induced by charge generation and recombination loss due to the suppressed charge-transfer (CT) state absorption. Despite a negligible driving force, all-PSC based on the polymer donor and acceptor combination with well-aligned energy levels exhibited efficient charge transfer and achieved an external quantum efficiency over 10% while maintaining a largeV(oc)of 1.02 V, leading to a 9.21% efficiency. Through various spectroscopy approaches, this work sheds light on the mechanism of energy loss in all-PSCs, which paves an avenue to achieving efficient all-PSCs with largeV(oc)and drives the further development of all-PSCs.
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