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Overcoming small-bandgap charge recombination in visible and NIR-light-driven hydrogen evolution by engineering the polymer photocatalyst structure
Designing an organic polymer photocatalyst for efficient hydrogen evolution in the near-infrared (NIR) light region is still a major challenge. The authors present here a series of polymer nanoparticles for a efficient hydrogen evolution under visible and NIR light irradiation, without combining or hybridizing with other materials.
- Mohamed Hammad Elsayed
- , Mohamed Abdellah
- & Ho-Hsiu Chou
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Highly stretchable polymer semiconductor thin films with multi-modal energy dissipation and high relative stretchability
Stretchable polymer semiconductors with high mechanical and electrical properties are challenging to develop. Wu et al. show that reversible molecular ordering under strain important for performance optimization and relative stretchability can be used to compare the relative strain tolerance of materials.
- Hung-Chin Wu
- , Shayla Nikzad
- & Zhenan Bao
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Near-infrared-II photoacoustic imaging and photo-triggered synergistic treatment of thrombosis via fibrin-specific homopolymer nanoparticles
The near-infrared-II (NIR-II) window has shown great promise for in vivo imaging and therapy. Here, the authors integrate a homopolymer and thermo-sensitive nitric oxide prodrug into nanoparticles for long-wavelength NIR-II photoacoustic imaging and synergistic treatment in preclinical thrombosis models.
- Jianwen Song
- , Xiaoying Kang
- & Ji Qi
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Organic laser power converter for efficient wireless micro power transfer
Due to the adjustable bandgap, flexibility, absence of heavy metals and high power per weight, organic laser converters have unique advantages in wireless power transfer. Here, authors integrate organic laser power converters exhibiting efficiency over 36% at 660 nm with photon flux of 9.5 mW/cm2.
- Yafei Wang
- , Zhong Zheng
- & Jianhui Hou
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Mesitylated trityl radicals, a platform for doublet emission: symmetry breaking, charge-transfer states and conjugated polymers
Neutral π-radicals are potential emitters for optoelectronic devices due to the absence of energetically low-lying non-emissive states. Here, the authors report mesityl-substituted tris(2,4,6-trichlorophenyl)methyl radicals and achieve maximum device efficiency of 28% at a wavelength of 689 nm.
- Petri Murto
- , Rituparno Chowdhury
- & Hugo Bronstein
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Solution-processable polymers of intrinsic microporosity for gas-phase carbon dioxide photoreduction
This works presents a series of solution processable, conjugated polymers of intrinsic microporosity, which are used as photocatalysts for carbon dioxide reduction to carbon monoxide in the presence of hydrogen.
- Floriana Moruzzi
- , Weimin Zhang
- & Iain McCulloch
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Multi-chiral materials comprising metallosupramolecular and covalent helical polymers containing five axial motifs within a helix
The axial helical structure of supramolecular and covalent polymers provides communication mechanisms among monomer repeating units. Here, the authors present multi-helical materials comprising five axial motifs that combine information from both metallosupramolecular and covalent helical polymers
- Francisco Rey- Tarrío
- , Emilio Quiñoá
- & Félix Freire
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Visualizing the multi-level assembly structures of conjugated molecular systems with chain-length dependent behavior
A deep understanding of multi-level assembly structures of conjugated polymers is crucial for developing high performance conjugated polymers and optoelectronic devices, however, it remains a challenge. Here, the authors report the morphological evolution of multi-level assembly of a model system of isoindigo-based conjugated polymer.
- Yang-Yang Zhou
- , Yu-Chun Xu
- & Jian Pei
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Self-healable polymer complex with a giant ionic thermoelectric effect
Thermoelectric devices have received significant attention for energy generation owing to their unique advantages over traditional heat engines. Here, the authors developed a well performing stretchable and self-healable iono thermoelectric material by optimizing the thermophoresis of protons in a polymer complex PEDOT:PAAMPSA:PA polymer.
- Dong-Hu Kim
- , Zico Alaia Akbar
- & Sung-Yeon Jang
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Improved photovoltaic performance and robustness of all-polymer solar cells enabled by a polyfullerene guest acceptor
Fullerene acceptors typically suffer from undesirable segregation and dimerization. Here, the authors report a poly(fullerene-alt-xylene) acceptor as guest component to facilitate charge transfer and suppress charge recombination, achieving efficiency of 18% for ternary all-polymer solar cells.
- Han Yu
- , Yan Wang
- & Shangshang Chen
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Article
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The effect of residual palladium on the performance of organic electrochemical transistors
The optimization of organic mixed ionic-electronic conductor is critical to realize high performance organic electrochemical transistors. Here, the authors demonstrate the removal of residual palladium impurities to be the key factor to achieving a figure-of-merit of [μC*] of over 2000 V−1 cm−1 s−1.
- Sophie Griggs
- , Adam Marks
- & Iain McCulloch
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Spatially nanoconfined N-type polymer semiconductors for stretchable ultrasensitive X-ray detection
Wearable and skin-like X-ray detectors need intrinsic flexibility and high sensitivity. Here Guo et al. develop a stretchable n-type polymer semiconductor with aligned nanofiber networks which achieve photosensitivity of 1.52×10^4 μC Gyair^-1 cm^−2 and low detection limit of 37.7 nGyair s^-1.
- Yangshuang Bian
- , Kai Liu
- & Yunlong Guo
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Main-chain engineering of polymer photocatalysts with hydrophilic non-conjugated segments for visible-light-driven hydrogen evolution
The introduction of hydrophilic segments into the main-chain of polymer photocatalysts allows water to efficiently enter the interior through these hydrophilic segments, and results in effective water/polymer interfaces for hydrogen evolution.
- Chih-Li Chang
- , Wei-Cheng Lin
- & Ho-Hsiu Chou
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High performance polymerized small molecule acceptor by synergistic optimization on π-bridge linker and side chain
The modification of small molecule acceptor building block and π−bridge linker is effective to improve photovoltaic performance. Here, the authors replace linear with branched alkyl chains and introduce difluorene-substituted linker to realise all-polymer solar cells with efficiency of 17.24%.
- Guangpei Sun
- , Xin Jiang
- & Yongfang Li
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Controllable synthesis of conjugated microporous polymer films for ultrasensitive detection of chemical warfare agents
The high toxicity of nerve agents makes the development of fluorescence sensors with suitable limit of detection challenging. Here, the authors propose a sensor design based on a conjugated microporous polymer film for the detection of diethyl chlorophosphate, a substitute of Sarin, with low detection limit of 2.5 ppt.
- Wanqi Mo
- , Zihao Zhu
- & Bin Li
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Reactive oxygen species-responsive and Raman-traceable hydrogel combining photodynamic and immune therapy for postsurgical cancer treatment
Combined immune checkpoint blockade (ICB) and photodynamic therapies have huge potential but suffer from possible damage of the antibodies. Here, the authors create a ROS-responsive hydrogel that protects the ICB antibodies and allows for sustained co-delivery and demonstrate restrained regrowth of tumours in vivo.
- Yiyi Zhang
- , Sidan Tian
- & Liang Luo
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Precision cancer sono-immunotherapy using deep-tissue activatable semiconducting polymer immunomodulatory nanoparticles
To improve the specificity of immunotherapy, here the authors report the design of a semiconducting polymer immunomodulatory nanoparticle with sonodynamic process to remotely release immune-modulators for deep-tissue precision cancer sono-immunotherapy.
- Jingchao Li
- , Yu Luo
- & Ruiping Zhang
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Anomalous thermo-osmotic conversion performance of ionic covalent-organic-framework membranes in response to charge variations
The development of ionic membranes with a high charge population is critical for realizing efficient thermo-osmotic energy conversion. Here, the authors demonstrated that the thermo-osmotic energy conversion efficiency can be improved by increasing the membrane charge density but this enhancement only occurs within a narrow window.
- Weipeng Xian
- , Xiuhui Zuo
- & Qi Sun
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High-mobility semiconducting polymers with different spin ground states
Semiconducting polymers with high-spin at their neutral ground state are rarely reported. Here the authors synthesize three semiconducting polymers with different spin ground states and high hole/electron mobility, by appropriate choice of the building blocks’ singlet-triplet energy gap, spin distributions and solid-state interchain interactions.
- Xiao-Xiang Chen
- , Jia-Tong Li
- & Ting Lei
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Non-metallic T2-MRI agents based on conjugated polymers
The toxicity of heavy metals for MRI contrast agents is an issue. Here, the authors report on the development of conjugated polymers nanoparticles based on paramagnetic polypyrrole to generate T2 MRI contrast effects by changing the interactions between polarons and water protons.
- Qinrui Lin
- , Yuhong Yang
- & Zhengzhong Shao
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Nanoscale π-conjugated ladders
Increasing the rigidity of a macromolecule while maintaining solubility is challenging. Here, the authors demonstrate covalent connection of two rigid-rod polymer chains with stiff connectors, leading to rigid ladder structures with well-defined conjugated rails.
- Stefanie A. Meißner
- , Theresa Eder
- & Sigurd Höger
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Regio- and sequence-controlled conjugated topological oligomers and polymers via boronate-tag assisted solution-phase strategy
The topology of polymers could be carefully controlled if the monomers were to be well-defined in sequence and regiochemical linkage. Here the authors present a method to synthesize oligomers of controlled sequence and regiochemistry, formed through iterative liquid-phase boronate-tagged syntheses, which are precursors to topologically distinct polymers.
- Chaoran Xu
- , Congze He
- & Xiangcheng Pan
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Approaching disorder-tolerant semiconducting polymers
In conjugated polymers, n-doping is often limited by the tradeoff between doping efficiency and charge carrier mobilities, since dopants often randomly distribute within polymers, leading to significant structural and energetic disorder. Here, the authors screen a large number of polymer building block combinations and explore the possibility of designing n-type conjugated polymers with good tolerance to dopant-induced disorder.
- Xinwen Yan
- , Miao Xiong
- & Ting Lei
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Self-assembly using a retro Diels-Alder reaction
Despite their great utility in synthetic and materials chemistry, Diels-Alder and retro Diels-Alder reactions have been vastly unexplored in promoting self-assembly processes. Here the authors show the release of steric bulkiness associated with a bridged bicyclic Diels Alder adduct by the retro Diels-Alder reaction that allowed generation of two building blocks that spontaneously self-assembled to form a supramolecular polymer.
- Jaeyoung Park
- , Jung-Moo Heo
- & Jong-Man Kim
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PEG-stabilized coaxial stacking of two-dimensional covalent organic frameworks for enhanced photocatalytic hydrogen evolution
Two-dimensional covalent organic frameworks are expected to boost photocatalytic H2 evolution from water splitting, but are not stable in photocatalysis. Here, authors demonstrate that photocatalytic performances can be enhanced by stabilizing layered stacking via a polymer-infiltration strategy.
- Ting Zhou
- , Lei Wang
- & Jia Guo
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Semi-conducting 2D rectangles with tunable length via uniaxial living crystallization-driven self-assembly of homopolymer
Semi-conducting two-dimensional polymer nanoobjects are promising materials but examples of self-assembled 2D nanosheets with controlled dimensions has not been shown before. Here, the authors precisely tune the length of 2D sheets of conjugated polymers by using blending, heating, and seeded-growth strategies.
- Sanghee Yang
- , Sung-Yun Kang
- & Tae-Lim Choi
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A high-conductivity n-type polymeric ink for printed electronics
The development of n-type conductive polymer inks is critical for the development of next-generation opto-electronic devices that rely on efficient hole and electron transport. Here, the authors report an alcohol-based, high performance and stable n-type conductive ink for printed electronics.
- Chi-Yuan Yang
- , Marc-Antoine Stoeckel
- & Simone Fabiano
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Orthogonal photochemistry-assisted printing of 3D tough and stretchable conductive hydrogels
3D-printing tough conductive hydrogels (TCHs) with complex structures is still a challenging task due to their inherent contrasting multinetworks, uncontrollable and slow polymerization. Here the authors show an orthogonal photochemistry-assisted printing strategy to make 3D TCHs in one pot.
- Hongqiu Wei
- , Ming Lei
- & You Yu
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90% yield production of polymer nano-memristor for in-memory computing
Though polymer memristors are promising for low‐power flexible edge computing applications, realizing efficient nanometer‐scale arrays remains a challenge. Here, the authors report a record high 90% production yield in nm‐scale 2D conjugated polymer memristors with homogeneous resistive switching.
- Bin Zhang
- , Weilin Chen
- & Yu Chen
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Predicting wavelength-dependent photochemical reactivity and selectivity
Predicting the conversion and selectivity of a photochemical reactions is challenging. Here, the authors introduce a framework for the quantitative prediction of the time-dependent progress of a photoligation reaction and predict LED-light induced conversion through a wavelength-resolved numerical simulation.
- Jan P. Menzel
- , Benjamin B. Noble
- & Christopher Barner-Kowollik
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A thermally activated and highly miscible dopant for n-type organic thermoelectrics
Realizing efficient n-doping in organic thermoelectrics remains a challenge due to dopant-semiconductor immiscibility, poor dopant stability and low doping efficiency. Here, the authors use computer-assisted screening to develop n-dopants for thermoelectric polymers that show record power factors.
- Chi-Yuan Yang
- , Yi-Fan Ding
- & Jian Pei
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Water stable molecular n-doping produces organic electrochemical transistors with high transconductance and record stability
Improving electron transport and stability of n-type organic electrochemical transistors (OECTs) is required to realize a commercially-viable technology for bioelectronics applications. Here, the authors report water-stable doped n-type OECTs with enhanced transconductance and record stability.
- Alexandra F. Paterson
- , Achilleas Savva
- & Sahika Inal
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A solution-processable and ultra-permeable conjugated microporous thermoset for selective hydrogen separation
Rigidity, as seen in crosslinked polymers, and plastic processability are mutually exclusive properties. Here, the authors prepare a solution-processable conjugated microporous thermoset with permanent pores and demonstrate its application as a two-dimensional molecular sieving membrane for hydrogen separation.
- Wei Liu
- , Shu-Dong Jiang
- & Kian Ping Loh
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Universal three-dimensional crosslinker for all-photopatterned electronics
To enable the large-area manufacture of solution-processed organic electronics, direct photocrosslinking processes has emerged as a promising technology solution. Here, the authors report an efficient universal crosslinking agent for micropatterning of stacked multi-layered organic electronics.
- Min Je Kim
- , Myeongjae Lee
- & Jeong Ho Cho
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Highly enantioselective photo-polymerization enhanced by chiral nanoparticles and in situ photopatterning of chirality
Chiral nanoparticles are capable of ultrasensitive detection, characterization, and asymmetric synthesis of chiral organic and biological molecules. Here, the authors use silver nanoparticles modified with cysteine, as the sole chiral source, and unpolarized UV light, to form polydiacetylene with high chiral asymmetry from achiral diacetylene monomers.
- Chenlu He
- , Zeyu Feng
- & Gang Zou
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Polydiacetylene-based ultrastrong bioorthogonal Raman probes for targeted live-cell Raman imaging
Raman probes which operate in the cellular silent region are of interest for live cell imaging. Here, the authors report on the development of a water soluble polydiacetylene Raman probe with enhanced Raman signal in the silent region which can be functionalised for organelle targeting and demonstrate application.
- Sidan Tian
- , Haozheng Li
- & Liang Luo
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Template-controlled on-surface synthesis of a lanthanide supernaphthalocyanine and its open-chain polycyanine counterpart
Extending the π‐conjugation of phthalocyanine dyes, while synthetically challenging, has the potential to produce desirable new molecular materials. Here, the authors use a templated on‐surface approach to synthesize several extended phthalocyanine derivatives from the same building block, including a lanthanide superphthalocyanine and an open‐chain polycyanine.
- Qitang Fan
- , Jan-Niclas Luy
- & J. Michael Gottfried
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Engineering crystalline quasi-two-dimensional polyaniline thin film with enhanced electrical and chemiresistive sensing performances
Large area and homogeneous PANI thin films are important in high-performance organic electronics, but controlling the thickness and crystallinity in PANI thin films is challenging. Here the authors use air-water interface and surfactant monolayer templates to synthesize large area crystalline PANI films with tunable thickness.
- Tao Zhang
- , Haoyuan Qi
- & Xinliang Feng
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| Open Access
Impact of polymorphism on the optoelectronic properties of a low-bandgap semiconducting polymer
Tuning polymorphism of conjugated polymers, though a promising method for studying and controlling the structure-property relations in these materials remains a challenge. Here, the authors identify two aggregated semi-crystalline polymorphs of a low-bandgap diketopyrrolopyrrole-based polymer.
- Mengmeng Li
- , Ahmed Hesham Balawi
- & René A. J. Janssen
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| Open Access
Two-dimensional semiconducting covalent organic frameworks via condensation at arylmethyl carbon atoms
Semiconducting covalent organic frameworks (COF) with conjugated structures are desired for optoelectric conversion but poor reversibility of bond forming reactions hampers the formation of crystalline structures. Here, the authors synthesise COFs with disubstituted C = C linkages which enable water splitting under visible light irradiation.
- Shuai Bi
- , Can Yang
- & Fan Zhang
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| Open Access
Facile syntheses of conjugated polymers for photothermal tumour therapy
Conjugated polymers are of interest for photothermal applications; however, synthesis of these polymers can be complex. Here, the authors report on a facile synthesis method that uses a modified CBT-Cys click reaction to make conjugated polymers and test these polymers for photothermal therapy applications.
- Peiyao Chen
- , Yinchu Ma
- & Gaolin Liang
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| Open Access
Redox gated polymer memristive processing memory unit
Though designing conductive polymers for memory devices is attractive for future low-cost flexible electronics, a proof-of-concept device has yet to be realized. Here, the authors report a redox-gated polymer memristive processing unit with programmable multilevel storage and logic functionalities.
- Bin Zhang
- , Fei Fan
- & Yu Chen
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| Open Access
Understanding structure-activity relationships in linear polymer photocatalysts for hydrogen evolution
While inorganic semiconductors are well-studied for their solar-to-fuel energy conversion abilities, organic materials receive far less attention. Here, authors prepare linear conjugated polymers as H2 evolution photocatalysts and rationalize photocatalytic activities with fundamental properties.
- Michael Sachs
- , Reiner Sebastian Sprick
- & Andrew I. Cooper
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| Open Access
Stepwise heating in Stille polycondensation toward no batch-to-batch variations in polymer solar cell performance
Polymer electronics may have a bright future but the poor reproducibility limits the scaled-up manufacturing. Here Lee et al. employ a stepwise-heating protocol in the Stille polycondensation and fabricate polymer solar cells with improved performance and ignorable device-to-device variations.
- Sang Myeon Lee
- , Kwang Hyun Park
- & Changduk Yang
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| Open Access
Sulfenate anions as organocatalysts for benzylic chloromethyl coupling polymerization via C=C bond formation
Polymerization reactions are often catalysed by metal compounds and hence there are concerns surrounding toxicity, cost and environmental friendliness. Here the authors show sulfenate anions as organocatalysts for benzylic chloromethyl-coupling polymerization reactions to form poly(stilbene)s.
- Minyan Li
- , Simon Berritt
- & Patrick J. Walsh
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Chiral induction in covalent organic frameworks
Controlling chirality and function in metal organic frameworks has been an achievement, but very difficult to carry out in covalent organic frameworks. Here the authors show chiral covalent organic frameworks that are crystallized from achiral precursors by chiral catalytic induction.
- Xing Han
- , Jie Zhang
- & Yong Cui
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| Open Access
Copper-surface-mediated synthesis of acetylenic carbon-rich nanofibers for active metal-free photocathodes
While photoelectrochemical devices combine light-absorption with fuel and electricity generation, their implementation is hampered by high costs and low output. Here, the authors synthesized acetylene-rich carbon fibers by copper-mediated polymerization for high-activity, metal-free photocathodes.
- Tao Zhang
- , Yang Hou
- & Xinliang Feng
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| Open Access
Uniform two-dimensional square assemblies from conjugated block copolymers driven by π–π interactions with controllable sizes
Crystallization-driven processes play a vital role in preparing 2D nanostructures which makes structures with high symmetry hard to access. Here the authors present a non-crystallization approach which is based on π–π interactions of a copolymer for the fabrication of 2D symmetric structures with good dimensional control.
- Liang Han
- , Meijing Wang
- & Feng He
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| Open Access
A low cost and high performance polymer donor material for polymer solar cells
A problem that hinders the commercialization of polymer solar cells is the complication in synthesis and thus the low yield and high cost of the polymers. Here, Sun et al. synthesize a new polymer via a two-step process with a yield close to 90% and show high photovoltaic performance with efficiency of 12%.
- Chenkai Sun
- , Fei Pan
- & Yongfang Li
Tuning polymer-backbone coplanarity and conformational order to achieve high-performance printed all-polymer solar cells