Selenophene Substitution Enabled High‐Performance n‐Type Polymeric Mixed Ionic‐Electronic Conductors for Organic Electrochemical Transistors and Glucose Sensors

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(1)

Published: Nov. 14, 2023

Abstract High‐performance n‐type polymeric mixed ionic‐electronic conductors (PMIECs) are essential for realizing organic electrochemical transistors (OECTs)‐based low‐power complementary circuits and biosensors, but their development still remains a great challenge. Herein, by devising two novel polymers (f‐BTI2g‐SVSCN f‐BSeI2g‐SVSCN) containing varying selenophene contents together with thiophene‐based counterpart as the control, it is demonstrated that gradually increasing loading in polymer backbones can simultaneously yield lowered lowest unoccupied molecular orbital levels, boosted charge‐transport properties, improved ion‐uptake capabilities. Therefore, remarkable volumetric capacitance ( C *) of 387.2 F cm −3 state‐of‐the‐art OECT electron mobility µ e,OECT ) 0.48 2 V −1 s synchronously achieved f‐BSeI2g‐SVSCN having highest content, yielding an unprecedented geometry‐normalized transconductance g m,norm 71.4 S record figure merit µC value 191.2 OECTs. Thanks to such excellent performance f‐BSeI2g‐SVSCN‐based OECTs, glucose sensor remarkably low detection limit 10 nM m decent selectivity further implemented, demonstrating power substitution strategy enabling high‐performance PMIECs biosensing applications.

Language: Английский

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High‐Performance and Ecofriendly Organic Thermoelectrics Enabled by N‐Type Polythiophene Derivatives with Doping‐Induced Molecular Order

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(8)

Published: Dec. 5, 2023

The ability of n-type polymer thermoelectric materials to tolerate high doping loading limits further development conductivity. Herein, two alcohol-soluble polythiophene derivatives that are n-PT3 and n-PT4 reported. Due the polymers more significantly than 100 mol%, both achieve electrical conductivity >100 S cm

Language: Английский

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Cyano‐Functionalized Pyrazine: A Structurally Simple and Easily Accessible Electron‐Deficient Building Block for n‐Type Organic Thermoelectric Polymers

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(11)

Published: Jan. 24, 2024

Abstract Developing low‐cost and high‐performance n‐type polymer semiconductors is essential to accelerate the application of organic thermoelectrics (OTEs). To achieve this objective, it critical design strong electron‐deficient building blocks with simple structure easy synthesis, which are for development semiconductors. Herein, we synthesized two cyano‐functionalized highly blocks, namely 3,6‐dibromopyrazine‐2‐carbonitrile (CNPz) 3,6‐Dibromopyrazine‐2,5‐dicarbonitrile (DCNPz), feature structures facile synthesis. CNPz DCNPz can be obtained via only one‐step reaction three‐step reactions from cheap raw materials, respectively. Based on DCNPz, acceptor–acceptor (A–A) polymers, P(DPP‐CNPz) P(DPP‐DCNPz) successfully developed, featuring deep‐positioned lowest unoccupied molecular orbital (LUMO) energy levels, beneficial thin‐film transistors (OTFTs) OTEs performance. An optimal unipolar electron mobility 0.85 1.85 cm 2 V −1 s P(DPP‐DCNPz), When doped N ‐DMBI, show high electrical conductivities/power factors 25.3 S /41.4 μ W m K −2 , 33.9 /30.4 Hence, pyrazine represent a new class structurally simple, readily accessible block constructing

Language: Английский

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A Highly Conductive n-Type Conjugated Polymer Synthesized in Water

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(23), P. 15860 - 15868

Published: May 30, 2024

Poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) is a benchmark hole-transporting (p-type) polymer that finds applications in diverse electronic devices. Most of its success due to facile synthesis water, exceptional processability from aqueous solutions, and outstanding electrical performance ambient. Applications fields like (opto-)electronics, bioelectronics, energy harvesting/storage devices often necessitate the complementary use both p-type n-type (electron-transporting) materials. However, availability materials amenable water-based polymerization processing remains limited. Herein, we present novel method enabling direct yielding highly conductive, water-processable conjugated polymer, namely, poly[(2,2′-(2,5-dihydroxy-1,4-phenylene)diacetic acid)-stat-3,7-dihydrobenzo[1,2-b:4,5-b′]difuran-2,6-dione] (PDADF), with remarkable conductivity as high 66 S cm–1, ranking among highest for polymers processed using green solvents. The new PDADF also exhibits stability, maintaining 90% initial after 146 days storage air. Our synthetic approach, along it yields, promises significant advancements sustainable development organic

Language: Английский

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Anion Doping as a “Trigger” to Modulate Defect‐Tailored Dielectric Coupling for Ultrathin Microwave Absorber

Small, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 1, 2024

Abstract Anion doping engineering is recognized as a prospective strategy to adjust the electronic configuration and transport capacity of carbon‐based magnetoelectric hybrids optimize defects for modulation electromagnetic (EM) properties. This study effectively accomplishes an overwhelming enhancement in dielectric coupling between conduction polarization CuCo bimetallic/carbon system by employing situ (N, O)/ex (S, Se) defect strategies. The well‐designed lattice distortions are facilitated large atomic radii (Se) intercalated carbon skeleton bimetallic CuCo, which activate reinforcement dipole high‐frequency region. Interestingly, appropriate number vacancies acts “electron traps” accelerate local charge redistribution, endowing with extremely strong interactions interface‐induced polarization. It remarkable that ultra‐thin feature (1.8 mm) able achieve extraordinary microwave attenuation (‒56.1 dB). Additionally, specific upgrading anionic Se beneficially hinders development phonon transmission, conferring Cu 2 Se/CoSe /NC‐Se aerogel outstanding infrared stealth capabilities along inheriting advantages traditional (lightness, compressive/structural stability, hydrophobicity/anti‐corrosive properties). research offers distinctive perspectives on advanced design multifunctional absorbers complex environments.

Language: Английский

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Bis(benzoselenadiazol)ethane: A π‐Extended Acceptor‐Dimeric Unit for Ambipolar Polymer Transistors with Hole and Electron Mobilities Exceeding 10 cm² V⁻¹ s⁻¹

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(17)

Published: March 5, 2024

Abstract The lack of ambipolar polymers with balanced hole ( μ h ) and electron mobilities e >10 cm 2 V −1 s is the main bottleneck for developing organic integrated circuits. Herein, we show design synthesis a π‐extended selenium‐containing acceptor‐dimeric unit, namely benzo[ c ][1,2,5]selenadiazol‐4‐yl)ethane (BBSeE), to address this dilemma. In comparison its sulfur‐counterpart, BBSeE demonstrates enlarged co‐planarity, selective noncovalent interactions, polarized Se−N bond, higher affinity. successful stannylation offers great opportunity access acceptor‐acceptor copolymer pN‐BBSeE, which shows narrower band gap, lower‐lying lowest unoccupied molecular orbital level (−4.05 eV), degree backbone planarity. Consequently, pN‐BBSeE‐based transistors display an ideally transporting property 10.65 10.72 , respectively. To best our knowledge, simultaneous / values >10.0 are performances ever reported polymers. addition, pN‐BBSeE excellent shelf‐storage stability, retaining over 85 % initial mobility after two months storage. Our study promising acceptor building block constructing high‐performance applied in next‐generation circuit.

Language: Английский

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Recent developments in polymer semiconductors with excellent electron transport performances

Chemical Society Reviews, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

This review describes the design considerations, bonding modes between monomers, structural modification strategies, and applications of polymer semiconductors with excellent electron transport performances.

Language: Английский

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Designer Conjugation-Break Spacer That Boosts Charge Transport in Semiconducting Terpolymers

Macromolecules, Journal Year: 2024, Volume and Issue: 57(12), P. 5902 - 5914

Published: June 5, 2024

Conjugated polymers (CPs) are pivotal for high-mobility applications, typically avoiding nonconjugated units due to their perceived negative impact on charge transport. Contrary this belief, our study introduces a unit, DKPDO, which when employed as conjugation-break spacer (CBS), significantly enhances DKPDO was obtained center-modified isoindigo variant featuring strongly electron-withdrawing amide groups that diminish the electron density and foster multiple hydrogen-bonding interactions. This results in enhanced deficiency reinforced coplanarity relative isoindigo. incorporated into polymer backbone, comprising bithiophene, create series of terpolymers with varied molar ratios, allowing systematic evaluation solubilities, interchain interactions, crystallinities, energy levels. Notably, incorporating universal improvement hole mobilities operational stabilities over DKPDO-free counterpart. Remarkably, terpolymer containing 2.5% achieves high mobility 4.12 cm2 V–1 s–1, approximately 6-fold higher than parent CP among highest CPs based center-inserted units. The not only, first time, realizes transport enhancement CBS backbones but also sets precedent strategic use developing high-performing CPs.

Language: Английский

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A High‐Mobility n‐Type Noncovalently‐Fused‐Ring Polymer for High‐Performance Organic Thermoelectrics

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(35)

Published: June 10, 2024

Conjugated polymers are emerging as competitive candidates for organic thermoelectrics (OTEs). However, to make the device truly pervasive, both p- and n-type conjugated essential. Despite great efforts, no equivalents p-type benchmark PEDOT:PSS exist date mainly due low electrical conductivity (σ). Herein, a near-amorphous polymer, namely pDFSe, is reported with high σ by achieving synergy between charge transport doping efficiency. The polymer pDFSe synthesized based on an acceptor-triad moiety of diketopyrrolopyrrole-difluorobenzoselenadiazole-diketopyrrolopyrrole (DFSe), which has noncovalently-fused-ring structure reinforce backbone rigidity. Furthermore, axisymmetric thiophene-selenophene-thiophene donor introduced, enables formation microstructures. above merits ensure good efficiency without scarifying efficient intrachain charge-carrier transport. Thus, pDFSe-based transistors exhibit electron mobility up 6.15 cm

Language: Английский

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Multi‐Selenophene Incorporated Thiazole Imide‐Based n‐Type Polymers for High‐Performance Organic Thermoelectrics

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 63(3)

Published: Nov. 24, 2023

Abstract Developing polymers with high electrical conductivity ( σ ) after n‐doping is a great challenge for the advance of field organic thermoelectrics (OTEs). Herein, we report series thiazole imide‐based n‐type by gradually increasing selenophene content in polymeric backbone. Thanks to strong intramolecular noncovalent N⋅⋅⋅S interaction and enhanced intermolecular Se⋅⋅⋅Se interaction, increase content, show lowered LUMOs, more planar backbone, improved film crystallinity versus selenophene‐free analogue. Consequently, polymer PDTzSI−Se highest achieves champion 164.0 S cm −1 power factor 49.0 μW m K −2 when applied OTEs n‐doping. The value one donor‐acceptor OTE materials reported date. Our work indicates that substitution powerful strategy developing high‐performance incorporated imides offer an excellent platform enabling backbone coplanarity, deep‐lying LUMO mobility/conductivity.

Language: Английский

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