Article
Chemistry, Multidisciplinary
Yang Lu, Zi-Di Yu, Hio-Ieng Un, Ze-Fan Yao, Hao-Yang You, Wenlong Jin, Liang Li, Zi-Yuan Wang, Bo-Wei Dong, Stephen Barlow, Elena Longhi, Chong-an Di, Daoben Zhu, Jie-Yu Wang, Carlos Silva, Seth R. Marder, Jian Pei
Summary: A simple solution-based co-deposition method has been reported to achieve high conductivity n-doped polymers. These polymers exhibit surprising structural tolerance and excellent miscibility with commonly used n-dopants, allowing high concentrations and high mobility of charge carriers simultaneously, resulting in excellent electrical conductivity and thermoelectric performance.
ADVANCED MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Changshuai Dong, Sihui Deng, Bin Meng, Jun Liu, Lixiang Wang
Summary: Acceptor-acceptor (A-A) copolymerization is an effective strategy to develop high-performance n-type conjugated polymers. By synthesizing a strong electron-deficient BNBP monomer, A-A type conjugated polymers with ultralow LUMO energy levels were successfully developed via Stille polycondensation, showing promising thermoelectric properties. This demonstrates the great potential of A-A type organoboron polymers for high-performance n-type thermoelectrics.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Xiaokang Geng, Tian Du, Chenhui Xu, Yingying Liu, Yunfeng Deng, Yanhou Geng
Summary: In this study, two conjugated polymers (CPs) were synthesized to obtain p-type and n-type conductive materials through selective doping. PTQDPP-2FT performed better in organic thermoelectric devices, with p-type and n-type power factors of 278.2 and 2.37 mu W m(-1) K-2, respectively. These are the best bipolar (p-type and n-type) performances achieved by selective doping of a single polymer.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Engineering, Environmental
Ji Min Han, Sang Eun Yoon, Ku Hyun Jung, Onyu Bae, Donguk Kim, Unjeong Kim, Hyungtak Seo, Felix Sunjoo Kim, Ki Chul Kim, Jong H. Kim, Bong-Gi Kim
Summary: This study synthesized a new conjugated polymer with efficient doping using both electron acceptor and Lewis acid type dopants, achieving high electrical conductivities. The interaction between the electron-donating atoms in the doped polymer and the dopants influenced the conductive properties and stability.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Chemistry, Multidisciplinary
Jian Liu, Gang Ye, Hinderikus G. O. Potgieser, Marten Koopmans, Selim Sami, Mohamad Insan Nugraha, Diego Rosas Villalva, Hengda Sun, Jingjin Dong, Xuwen Yang, Xinkai Qiu, Chen Yao, Giuseppe Portale, Simone Fabiano, Thomas D. Anthopoulos, Derya Baran, Remco W. A. Havenith, Ryan C. Chiechi, L. Jan Anton Koster
Summary: The use of amphipathic side chains in an n-type donor-acceptor copolymer selectively increases the Seebeck coefficient and improves the power factor by a factor of approximately 5. The alkyl spacer reduces energetic disorder, controls dopant sites, and minimizes the adverse influence of counterions. This molecular strategy optimizes the Seebeck coefficient and offers a new approach to improving n-type polymeric thermoelectrics by optimizing dopant location.
ADVANCED MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Eui Hyun Suh, Sang Beom Kim, Han Sol Yang, Jaeyoung Jang
Summary: This study demonstrates the feasibility of modulating doping mechanisms by utilizing the competitive interactions between BCF and H2O or Lewis basic groups in polymers. Polymers without strong Lewis basic groups undergo Bronsted acid doping, leading to the formation of delocalized free charge carriers and superior thermoelectric properties. However, polymers with strong Lewis basic groups undergo both doping mechanisms competitively, resulting in decreased thermoelectric properties. Nevertheless, the reduced thermoelectric properties can be improved by thermal annealing.
ADVANCED FUNCTIONAL MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Jiwoo Min, Jaemin Im, Seung Hyun Kim, Hyun Ho Choi, Kilwon Cho
Summary: Molecular doping affects the charge transport pathways and mechanisms in conjugated polymer thin films, and this is highly attributed to the initial molecular ordering of the films. The study reveals the differences in coherent and incoherent charge transport and the impact of chemical structure on the charge transport performance.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Review
Polymer Science
Suhao Wang, Guangzheng Zuo, Jongho Kim, Henning Sirringhaus
Summary: Thanks to the combined efforts of scientists in various research fields, there have been significant advancements in the past decade in the application of conjugated polymers as thermoelectric materials. However, there is a lack of systematic evaluations on the impact of molecular design on thermoelectric properties. A comprehensive understanding of the relationship between molecular structure and thermoelectric properties will facilitate the rational design of next-generation thermoelectric polymers.
PROGRESS IN POLYMER SCIENCE
(2022)
Article
Chemistry, Multidisciplinary
Junhui Tang, Jingjing Ji, Ruisi Chen, Yongkun Yan, Yan Zhao, Ziqi Liang
Summary: In this study, a series of D-A semiconducting copolymers with various electron-deficient A-units were systematically investigated for efficient OTEs. The relationship between thermoelectric characteristics and the electron-withdrawing ability of A-unit was elucidated through p-type doping, highlighting the importance of the strong D-A nature and highly electron-deficient A-unit in enhancing Seebeck coefficient while impacting doping efficiency and electrical conductivity. Ultimately, a high peak power factor and outstanding Seebeck coefficient were achieved in a paradigm OPV donor, demonstrating great potential in wearable electronics driven by a small temperature gradient.
Article
Engineering, Environmental
Hansol Lee, Su Bin Lee, Young -Shin Kim, Hoimin Kim, Min -Jae Kim, Tae Woong Yoon, Dongki Lee, Jeong Ho Cho, Yun-Hi Kim, Boseok Kang
Summary: The effect of molecular structure on the microstructure and thermoelectric properties of donor-acceptor-type conjugated polymers based on isoindigo (IID) unit was investigated. The crystallinity and molecular packing of the polymers were found to change significantly depending on the symmetry of the donor unit copolymerized with the IID unit, resulting in differences in the doping and charge transport characteristics. A polymer with high crystallinity and fibril-like crystalline network showed excellent thermoelectric performance due to its highly ordered structure, exhibiting a high power factor of 212 μWm-1K-2 upon doping. This study demonstrates the potential of IID unit as a promising building block for high-performance conjugated polymers for thermoelectric applications and provides important guidelines for the design of IID-based polymers with high thermoelectric performance.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Physical
Duckhyun Ju, Jimin Kim, Hyunwoo Yook, Jeong Woo Han, Kilwon Cho
Summary: Researchers systematically controlled the counter-ion-induced disorder in PEDOT using a counter-ion exchange method and analyzed how the disorder affected the TE transport properties of the polymer.
Article
Polymer Science
Hansol Lee, Huan Li, Young-Shin Kim, Sang Min Park, Dongki Lee, Sungjoo Lee, Hwa Sung Lee, Yun-Hi Kim, Boseok Kang
Summary: This study synthesized three novel conjugated polymers based on DTP and compared their thermoelectric properties. One of the copolymers, DPP-MeDTP, exhibited higher electrical conductivity and thermoelectric power factor, attributed to its highly planar molecular structure and crystalline order.
MACROMOLECULAR RAPID COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Jimin Kim, Duckhyun Ju, Seunghyun Kim, Kilwon Cho
Summary: A disorder-tolerant doping strategy that can greatly suppress dopant-induced structural and energetic disorder of conjugated polymers (CPs) is demonstrated using a promising molecular dopant, tris(pentafluorophenyl)borane. Under a non-polar aliphatic solvent, dopants effectively infiltrate into CP films and enable high solid-state ordering even after a large amount of charge carrier generation, resulting in highly delocalized transport properties with remarkable thermoelectric performance.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Review
Physics, Multidisciplinary
Qi Zhang, Hengda Sun, Meifang Zhu
Summary: This review discusses the performance and factors affecting n-type organic thermoelectric (OTE) materials, with a focus on the effect of backbone planarity on doping efficiency and thermoelectric performance. Strategies for improving performance, such as implementing rigid backbones or modifying conventional building blocks, are summarized. The outlook section highlights new possibilities for the future development of this field.
Article
Chemistry, Physical
Pablo Durand, Huiyan Zeng, Till Biskup, Vishnu Vijayakumar, Viktoriia Untilova, Celine Kiefer, Benoit Heinrich, Laurent Herrmann, Martin Brinkmann, Nicolas Leclerc
Summary: Combining side chain engineering and controlled alignment of PBTTT can produce oriented thin films with improved thermoelectric performance when doped sequentially with F(6)TCNNQ. The substitution of linear alkyl side-chains with slightly polar n-C7OC4 leads to enhanced structural order and thermo-mechanical properties. The combination of improved alignment and random orientation of intercalated F(6)TCNNQ dopants helps reach a very high charge conductivity and a record power factor in the polymer chain direction.
ADVANCED ENERGY MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Malgorzata Nguyen, Ulrike Kraft, Wen Liang Tan, Illia Dobryden, Katharina Broch, Weimin Zhang, Hio-Ieng Un, Dimitrios Simatos, Deepak Venkateshavaran, Iain McCulloch, Per M. Claesson, Christopher R. McNeill, Henning Sirringhaus
Summary: Conjugated polymer field-effect transistors show excellent mechanical properties, high charge-carrier mobilities, and compatibility with large-area, low-temperature processing, making them a promising technology for flexible electronics. However, their electrical stability is still a concern. This study presents a simple method of antisolvent treatment to improve the stability and performance of solution-processable indacenodithiophene-co-benzothiadiazole (IDT-BT) polymer transistors. The method increases the degree of crystallinity in the weakly crystalline polymer films, reducing electron trapping and charge traps. This highlights the importance of microstructure in weakly crystalline polymer films and offers a processing strategy for reliable flexible electronics.
ADVANCED MATERIALS
(2023)
Article
Polymer Science
Doan Vu, Wen Liang Tan, Lu He, Alexander Ehm, Dietrich R. T. Zahn, Christopher R. McNeill
Summary: We report the discovery of a third crystalline polymorph of the electron-transporting conjugated polymer P(NDI2OD-T2), called form III, which exhibits an end-on texture. This new polymorph is characterized by the incorporation of two monomer units along the backbone-stacking direction, resulting in a doubling of the unit cell c axis. The formation of form III crystallites is achieved by melt annealing a thin film followed by slow cooling. Analysis using grazing-incidence wide-angle X-ray scattering (GIWAXS) and peak simulation confirms the unique packing of this polymorph. This discovery presents an exciting opportunity to study the structure/function relationships of this important semiconducting polymer.
Article
Chemistry, Physical
Lucas Q. Flagg, Jonathan W. Onorato, Christine K. Luscombe, Vinayak Bhat, Chad Risko, Ben Levy-Wendt, Michael F. Toney, Christopher R. McNeill, Guillaume Freychet, Mikhail Zhernenkov, Ruipeng Li, Lee J. Richter
Summary: Organic mixed ionic-electronic conductors (OMIECs) have the potential for various new technologies, but their complex behavior inhibits material design. This report presents the use of RXRD to determine the structure of a doped polymer OMIEC. The insights from RXRD provide important information on ion location and doping behavior, contributing to a better understanding of transport in OMIECs.
CHEMISTRY OF MATERIALS
(2023)
Article
Materials Science, Multidisciplinary
Clemens Matt, Rukiya Matsidik, Deborah L. Meyer, Mirjam Schroeder, Michael Sommer, Till Biskup
Summary: Semiconducting polymers hold great promise in revolutionizing electronic device manufacturing and deployment for various applications. Conjugated push-pull copolymers, consisting of alternating donor and acceptor moieties, are crucial in these applications due to their highly tunable electronic structure. Understanding the electronic structure of these materials is essential for a detailed understanding of their structure-function relationship in organic electronics. Spectroscopic tools, like time-resolved electron paramagnetic resonance (TREPR), are of utmost importance in providing molecular resolution and discriminating between different repeat units to determine the actual representation of the polymer's electronic structure. In this study, TREPR spectroscopy was used to identify the repeat unit NDI-T2 as the representative structure for the polymer PNDIT2, while the alternative building block T-NDI-T had a distinct electronic structure. These results are highly important for the rational design of conjugated polymers in organic electronics applications.
ORGANIC ELECTRONICS
(2023)
Article
Chemistry, Physical
Carola S. Seelmann, Simona G. Huwiler, Martin Culka, Marc J. F. Strampraad, Till Biskup, Stefan Weber, G. Matthias Ullmann, Volker Schunemann, Peter-Leon Hagedoorn, Antonio J. Pierik, Matthias Boll
Summary: In anaerobic aromatic compound degrading microbes, class II benzoyl-coenzyme A (CoA) reductases (BCRs) reduce benzoyl-CoA to cyclohexa-1,5-diene-1-carboxyl-CoA (1,5-dienoyl-CoA) through a tungsten-bis-metallopterin (MPT) cofactor. This study provides experimental evidence for the Birch-like reduction mechanism via W(V)/radical intermediates and reveals the unique tetrahydro state of MPT cofactors essential for the reversibility of enzymatic Birch reduction.
Article
Chemistry, Physical
Leonardo Lamanna, Giuseppina Pace, Pietro Cataldi, Fabrizio Viola, Marco Friuli, Valerio Galli, Christian Demitri, Mario Caironi
Summary: Edible electronics that can be safely ingested and degraded in the human body have various applications, such as sensing physiological parameters, tagging food, and developing edible actuators. Ethylcellulose and activated carbon composites have been proposed as suitable materials for energy harvesting and storage in these edible devices. The combination of these materials allows for the production of bi-layered films with insulating top layers and low electrical resistivity at the bottom, enabling the successful operation of electropositive elements in organic triboelectric nanogenerators and electrodes in fully edible supercapacitors. These edible devices demonstrate potential for future applications in energy generation and storage.
Article
Chemistry, Multidisciplinary
Mengting Jiang, Stefano Pecorario, Nicolas F. F. Zorn, Jana Zaumseil, Mario Caironi
Summary: Solution-processed networks of semiconducting single-walled carbon nanotubes (SWCNTs) have potential applications in digital circuits, thermoelectric devices, and healthcare. Charge modulation microscopy (CMM) is used to study charge transport in field-effect transistors (FETs) based on different types of SWCNT networks, providing insights into the spatial distribution and evolution of free carriers during FET switching. The results show that preferential percolation paths are responsible for the transportation of holes and electrons, and the SWCNT density and band gap influence the charge density and transport paths.
ADVANCED MATERIALS INTERFACES
(2023)
Editorial Material
Chemistry, Physical
Annamaria Petrozza, Mario Caironi
ACS ENERGY LETTERS
(2023)
Article
Energy & Fuels
Xin Li, Chengyi Xiao, Zhaofan Yang, Hao Wang, Baiqiao Liu, Wen Liang Tan, Qiaomei Chen, Chao Wang, Christopher R. McNeill, Weiwei Li
Summary: In this study, three double-cable conjugated polymers were developed for indoor single-component organic solar cells (SCOSCs). The new polymers have pendent nonfused electron acceptors with A-pi-D-pi-A configuration, using 1H-indene-1,3(2H)-dione (ID) as an electron-withdrawing end group in group A. These polymers show absorption spectra in the range of 400-700 nm, matching the spectra of indoor LED lights. Additionally, the introduction of ID units and halogen atoms enables the polymers to exhibit high photovoltage (>1.0 V) in SCOSCs, resulting in a high efficiency of 18% under indoor light illumination. This research provides a novel modular design approach for wide-bandgap double-cable conjugated polymers that can be used for indoor photovoltaics.
Article
Nanoscience & Nanotechnology
Zhijie Hu, Chao Wang, Yikun Wang, Baiqiao Liu, Shijie Liang, Chengyi Xiao, Christopher R. Mcneill, Weiwei Li
Summary: The invention of near-infrared pedant-based double-cable conjugated polymers has shown significant efficacy in single-component organic solar cells. These polymers exhibit broad absorption spectra and suitable energy levels. Fluorination of the polymers further enhances their performance, leading to decreased voltage losses and increased power conversion efficiencies in SCOSCs.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
Doan Vu, Linjing Tang, Lars Thomsen, Martyn Jevric, Mats R. Andersson, Christopher R. McNeill
Summary: In this study, the influence of molecular packing and orientation of conjugated polymer chains in thin films on the charge transport properties and device performance of polymer-based optoelectronic devices was extensively investigated. The effects of various processing conditions on the thin-film microstructure were studied using grazing-incidence wide-angle X-ray scattering. It was found that the recently discovered third crystalline form of a well-studied electron transporting polymer evolved directly from the face-on oriented form upon melting under specific conditions.
CHEMISTRY OF MATERIALS
(2023)
Article
Engineering, Electrical & Electronic
Ao Liu, Huihui Zhu, Sai Bai, Youjin Reo, Mario Caironi, Annamaria Petrozza, Letian Dou, Yong-Young Noh
Summary: Advancements in metal halide perovskite semiconductors have created renewed interest in their use in transistors. Improvements in performance have been made through fine-tuning of material compositions, processing techniques, and device engineering. However, more understanding is needed regarding the electrical properties of these materials, as well as their potential for use in large-area and microscale electronics.
NATURE ELECTRONICS
(2023)
Article
Energy & Fuels
Yahui Tang, Wen Liang Tan, Zhuping Fei, Martin Heeney, Christopher R. Mcneill
Summary: In order to understand the limitations of open-circuit voltage in organic solar cells, the energy levels of neat donor and acceptor samples are often characterized, but this may not reflect the energy levels at the donor:acceptor interface in blends. Organic semiconductors, especially non-fullerene acceptors, are sensitive to microstructural changes in thin films. This study investigates the differences in molecular packing between neat and blend films using temperature-dependent current-voltage measurements. The results show that the interfacial energy levels differ for different systems, highlighting the importance of considering microstructure-dependent differences when studying energy losses in non-fullerene acceptor organic solar cells.
Article
Chemistry, Multidisciplinary
Martina Rimmele, Zhuoran Qiao, Julianna Panidi, Francesco Furlan, Chulyeon Lee, Wen Liang Tan, Christopher R. McNeill, Youngkyoo Kim, Nicola Gasparini, Martin Heeney
Summary: The dramatic improvement of the PCE of organic photovoltaic devices has been driven by the development of new polymer donor materials and non-fullerene acceptors. A new approach was reported to introduce various solubilizing groups into a benzo[c][1,2,5]thiadiazole acceptor comonomer, allowing for the preparation of a library of donor polymers for rapid screening of properties and performance. The donor polymer FO6-T emerged as the optimal material, exhibiting good solubility and achieving high PCE, making it suitable for large-scale applications.
MATERIALS HORIZONS
(2023)
Article
Chemistry, Multidisciplinary
Dongdong Xia, Shengxi Zhou, Wen Liang Tan, Safakath Karuthedath, Chengyi Xiao, Chaowei Zhao, Frederic Laquai, Christopher R. McNeill, Weiwei Li
Summary: In this work, the preferential end-on orientation was obtained for the first time in a conjugated molecular dyad. The molecular orientation was shifted by introducing a fused-ring structure, resulting in higher charge carrier mobilities and better power conversion efficiency in organic solar cells.
