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1.
ACS Appl Mater Interfaces ; 11(36): 33173-33178, 2019 Sep 11.
Artigo em Inglês | MEDLINE | ID: mdl-31405281

RESUMO

In this work, position effects of an alkylthio side chain were investigated by designing and synthesizing two copolymers based on a phenyl-substituted benzo[1,2-b:4,5-b']dithiophene (BDTP) and difluorobenzotriazole (FTAZ). The polymer based on the meta-position-alkylthiolated BDTP, named m-PBDTPS-FTAZ, showed a relatively broader bandgap (2.00 vs 1.96 eV) and lower highest occupied molecular orbital (HOMO) energy level (-5.40 vs -5.32 eV) than its para-positioned structural isomeric analogue polymer (named p-PBDTPS-FTAZ), that is, m- and p-PBDTPS-FTAZ with the side chain structured as ethylhexyl- in the phenyl unit and hexyldecyl- in the FTAZ moiety. When blended with ITIC, m-PBDTPS-FTAZ showed a comparable crystallinity but more uniform morphology compared to that of p-PBDTPS-FTAZ. A high power conversion efficiency of 13.16% was achieved for m-PBDTPS-FTAZ:ITIC devices with a high open circuit voltage (VOC) of 0.95 V, which is higher than that of p-PBDTPS-FTAZ:ITIC devices (10.86%) with a VOC of 0.89 V. Therefore, m-BDTPS could be an effective donor unit to construct high-efficiency polymers due to its effectively decreased HOMO energy level of polymers while still maintaining good molecular stacking.

2.
Chem Asian J ; 14(18): 3085-3095, 2019 Sep 16.
Artigo em Inglês | MEDLINE | ID: mdl-31310451

RESUMO

Over the past decade, organic solar cells (OSCs) have achieved a dramatic boost in their power conversion efficiencies from about 6 % to over 16 %. In addition to developments in device engineering, innovative photovoltaic materials, especially fluorinated donors and acceptors, have become the dominant factor for improved device performance. This minireview highlights fluorinated photovoltaic materials that enable efficient OSCs. Impressive OSCs have been obtained by developing some important molds of fluorinated donor and acceptor systems. The molecular design strategy and the matching principle of fluorinated donors and acceptors in OSCs are discussed. Finally, a concise summary and outlook are presented for advances in fluorinated materials to realize the practical application of OSCs.


Assuntos
Técnicas Eletroquímicas , Compostos Orgânicos/química , Energia Solar , Halogenação , Processos Fotoquímicos
3.
Adv Mater ; 31(22): e1807019, 2019 May.
Artigo em Inglês | MEDLINE | ID: mdl-30701605

RESUMO

The development of conjugated alternating donor-acceptor (D-A) copolymers with various electron-rich and electron-deficient units in polymer backbones has boosted the power conversion efficiency (PCE) over 17% for polymer solar cells (PSCs) over the past two decades. However, further enhancements in PCEs for PSCs are still imperative to compensate their imperfect stability for fulfilling practical applications. Meanwhile development of these alternating D-A copolymers is highly demanding in creative design and syntheses of novel D and/or A monomers. In this regard, when being possible to adopt an existing monomer unit as a third component from its libraries, either a D' unit or an A' moiety, to the parent D-A type polymer backbones to afford conjugated D-A terpolymers, it will give a facile and cost-effective method to improve their light absorption and tune energy levels and also interchain packing synergistically. Moreover, the rationally controlled stoichiometry for these components in such terpolymers also provides access for further fine-tuning these factors, thus resulting in high-performance PSCs. Herein, based on their unique features, the recent progress of conjugated D-A terpolymers for efficient PSCs is reviewed and it is discussed how these factors influence their photovoltaic performance, for providing useful guidelines to design new terpolymers toward high-efficiency PSCs.

4.
Adv Mater ; 31(22): e1807275, 2019 May.
Artigo em Inglês | MEDLINE | ID: mdl-30790384

RESUMO

All-polymer solar cells (all-PSCs) based on n- and p-type polymers have emerged as promising alternatives to fullerene-based solar cells due to their unique advantages such as good chemical and electronic adjustability, and better thermal and photochemical stabilities. Rapid advances have been made in the development of n-type polymers consisting of various electron acceptor units for all-PSCs. So far, more than 200 n-type polymer acceptors have been reported. In the last seven years, the power conversion efficiency (PCE) of all-PSCs rapidly increased and has now surpassed 10%, meaning they are approaching the performance of state-of-the-art solar cells using fullerene derivatives as acceptors. This review discusses the design criteria, synthesis, and structure-property relationships of n-type polymers that have been used in all-PSCs. Additionally, it highlights the recent progress toward photovoltaic performance enhancement of binary, ternary, and tandem all-PSCs. Finally, the challenges and prospects for further development of all-PSCs are briefly considered.

5.
Elife ; 72018 12 13.
Artigo em Inglês | MEDLINE | ID: mdl-30543324

RESUMO

Inflammation often induces regeneration to repair the tissue damage. However, chronic inflammation can transform temporary hyperplasia into a fertile ground for tumorigenesis. Here, we demonstrate that the microRNA miR-34a acts as a central safeguard to protect the inflammatory stem cell niche and reparative regeneration. Although playing little role in regular homeostasis, miR-34a deficiency leads to colon tumorigenesis after Citrobacter rodentium infection. miR-34a targets both immune and epithelial cells to restrain inflammation-induced stem cell proliferation. miR-34a targets Interleukin six receptor (IL-6R) and Interleukin 23 receptor (IL-23R) to suppress T helper 17 (Th17) cell differentiation and expansion, targets chemokine CCL22 to hinder Th17 cell recruitment to the colon epithelium, and targets an orphan receptor Interleukin 17 receptor D (IL-17RD) to inhibit IL-17-induced stem cell proliferation. Our study highlights the importance of microRNAs in protecting the stem cell niche during inflammation despite their lack of function in regular tissue homeostasis.


Assuntos
Transformação Celular Neoplásica/genética , Colo/metabolismo , Infecções por Enterobacteriaceae/genética , Perfilação da Expressão Gênica , Inflamação/genética , MicroRNAs/genética , Animais , Células Cultivadas , Citrobacter rodentium/fisiologia , Colo/microbiologia , Colo/patologia , Infecções por Enterobacteriaceae/microbiologia , Inflamação/microbiologia , Masculino , Camundongos Endogâmicos C57BL , Camundongos Knockout , Camundongos Transgênicos , Células-Tronco Neoplásicas/metabolismo , Receptores de Interleucina/genética , Receptores de Interleucina/metabolismo , Células Th17/metabolismo
6.
Conf Proc IEEE Eng Med Biol Soc ; 2018: 5022-5025, 2018 07.
Artigo em Inglês | MEDLINE | ID: mdl-30441469

RESUMO

Classically, the Wnt/ß-catenin and Notch /Delta signaling pathways were thought to operate through separate mechanisms, performing distinct roles in tissue patterning. However, it has been shown that b-catenin activates transcription of Hesl, a signaling intermediate in the Notch /Delta pathway that controls its lateral inhibition mechanism. To investigate this non-canonical crosstalk mechanism, a new gene circuit, integrating the two pathways, is proposed and simulated in two-cell and multi-cell environments. This model also captures both Paneth cell- mediated and mesenchymal Wnt production. The simulations verify that the gene circuit is temporally bistable and capable of forming a pattern on a multi-cell grid. Last, the model exhibits a bifurcation based on the steady state concentration of Wnt and the relative amount of control b-catenin has over the Hesl promoter, providing a possible mechanism to explain why a homogeneous population of transit amplifying cells is observed directly above the more diverse stem niche.


Assuntos
Redes Reguladoras de Genes , Receptores Notch/genética , Fatores de Transcrição HES-1/metabolismo , Via de Sinalização Wnt , Simulação por Computador , Humanos , Modelos Biológicos , Celulas de Paneth/fisiologia , Regiões Promotoras Genéticas
7.
Adv Mater ; : e1706584, 2018 Jul 10.
Artigo em Inglês | MEDLINE | ID: mdl-29987856

RESUMO

Due to the so-called energy-gap law and aggregation quenching, the efficiency of organic light-emitting diodes (OLEDs) emitting above 800 nm is significantly lower than that of visible ones. Successful exploitation of triplet emission in phosphorescent materials containing heavy metals has been reported, with OLEDs achieving remarkable external quantum efficiencies (EQEs) up to 3.8% (peak wavelength > 800 nm). For OLEDs incorporating fluorescent materials free from heavy or toxic metals, however, we are not aware of any report of EQEs over 1% (again for emission peaking at wavelengths > 800 nm), even for devices leveraging thermally activated delayed fluorescence (TADF). Here, the development of polymer light-emitting diodes (PLEDs) peaking at 840 nm and exhibiting unprecedented EQEs (in excess of 1.15%) and turn-on voltages as low as 1.7 V is reported. These incorporate a novel triazolobenzothiadiazole-based emitter and a novel indacenodithiophene-based transport polymer matrix, affording excellent spectral and transport properties. To the best of knowledge, such values are the best ever reported for electroluminescence at 840 nm with a purely organic and solution-processed active layer, not leveraging triplet-assisted emission.

8.
Zhongguo Zhen Jiu ; 38(4): 391-7, 2018 Apr 12.
Artigo em Chinês | MEDLINE | ID: mdl-29696924

RESUMO

In this paper, scientific theory was used to prove that the meridian was the resonant channel of information energy of life, and experiment and demonstration was performed to reveal meridians to explore the significance of revealing meridian. Based on the theory of physics, biochemistry, molecular biology and information theory, the essence of meridian was demonstrated in theory. According to TCM meridian theory, acupuncture was applied at selected acupoints; the infrared thermograms of stomach meridian of foot yangming, large intestine meridian of hand yangming, small intestine meridian of hand taiyang, pericardium meridian of hand jueyin, heart meridian of hand shaoyin, triple energizer meridian of hand shaoyang, liver meridian of foot jueyin, bladder meridian of foot taiyang were recorded before and after acupuncture. As a result, thermogram recorded and showed the visual image of the meridian. It is indicated that an energy transmission network which cannot be dissected existing in the body, which was believed to be meridian. It was the resonant channel of information energy of life, and could be shown by thermogram. These experiments and theory have significance in science.


Assuntos
Acupuntura , Meridianos , Pontos de Acupuntura , Humanos
9.
ACS Appl Mater Interfaces ; 10(15): 12937-12946, 2018 Apr 18.
Artigo em Inglês | MEDLINE | ID: mdl-29589432

RESUMO

A conjugated donor-acceptor polymer, poly[4,4,9,9-tetrakis(4-hexylphenyl)-4,9-dihydro- s-indaceno[1,2- b:5,6- b']dithiophene-2,7-diyl- alt-5-(2-ethylhexyl)-4 H-thieno[3,4- c]pyrrole-4,6(5 H)-dione-1,3-diyl] (PIDT-TPD), is blended with the fullerene derivative [6,6]phenyl-C61-butyric acid methyl ester (PC61BM) for the fabrication of thin and solution-processed organic photodetectors (OPDs). Systematic screening of the concentration ratio of the blend and the molecular weight of the polymer is performed to optimize the active layer morphology and the OPD performance. The device comprising a medium molecular weight polymer (27.0 kg/mol) in a PIDT-TPD:PC61BM 1:1 ratio exhibits an external quantum efficiency of 52% at 610 nm, a dark current density of 1 nA/cm2, a detectivity of 1.44 × 1013 Jones, and a maximum 3 dB cutoff frequency of 100 kHz at -5 V bias. These results are remarkable among the state-of-the-art red photodetectors based on conjugated polymers. As such, this work presents a functional organic active material for high-speed OPDs with a linear photoresponse at different light intensities.

10.
Langmuir ; 33(45): 12859-12864, 2017 11 14.
Artigo em Inglês | MEDLINE | ID: mdl-29028341

RESUMO

Ferroelectric molecular compounds present great advantages for application in electronics because they combine high polarization values, comparable to those of inorganic materials, with the flexibility and low-cost properties of organic ones. However, some limitations to their applicability are related to the high crystallinity required to deploy ferroelectricity. In this article, highly ordered ferroelectric patterned thin films of diisopropylammonium bromide have been successfully fabricated by a lithographically controlled wetting technique. Confinement favors the self-organization of ferroelectric crystals, avoiding the formation of polymorphs and promoting the long-range orientation of crystallographic axes. Patterned structures present high stability, and the polarization can be switched to be arranged in stable domain pattern for application in devices.

11.
Ultramicroscopy ; 176: 23-30, 2017 05.
Artigo em Inglês | MEDLINE | ID: mdl-28341555

RESUMO

We show by in situ microscopy that the effects of electron beam irradiation during transmission electron microscopy can be used to lock microstructural features and enhance the structural thermal stability of a nanostructured polymer:fullerene blend. Polymer:fullerene bulk-heterojunction thin films show great promise for use as active layers in organic solar cells but their low thermal stability is a hindrance. Lack of thermal stability complicates manufacturing and influences the lifetime of devices. To investigate how electron irradiation affects the thermal stability of polymer:fullerene films, a model bulk-heterojunction film based on a thiophene-quinoxaline copolymer and a fullerene derivative was heat-treated in-situ in a transmission electron microscope. In areas of the film that exposed to the electron beam the nanostructure of the film remained stable, while the nanostructure in areas not exposed to the electron beam underwent large phase separation and nucleation of fullerene crystals. UV-vis spectroscopy shows that the polymer:fullerene films are stable for electron doses up to 2000kGy.

12.
Ultramicroscopy ; 173: 16-23, 2017 02.
Artigo em Inglês | MEDLINE | ID: mdl-27902941

RESUMO

We show by in situ microscopy that the effects of electron beam irradiation during transmission electron microscopy can be used to lock microstructural features and enhance the structural thermal stability of a nanostructured polymer:fullerene blend. Polymer:fullerene bulk-heterojunction thin films show great promise for use as active layers in organic solar cells but their low thermal stability is a hindrance. Lack of thermal stability complicates manufacturing and influences the lifetime of devices. To investigate how electron irradiation affects the thermal stability of polymer:fullerene films, a model bulk-heterojunction film based on a thiophene-quinoxaline copolymer and a fullerene derivative was heat-treated in-situ in a transmission electron microscope. In areas of the film that exposed to the electron beam the nanostructure of the film remained stable, while the nanostructure in areas not exposed to the electron beam underwent large phase separation and nucleation of fullerene crystals. UV-vis spectroscopy shows that the polymer:fullerene films are stable for electron doses up to 2000kGy.

13.
J Am Chem Soc ; 138(34): 10935-44, 2016 08 31.
Artigo em Inglês | MEDLINE | ID: mdl-27479751

RESUMO

Growing interests have been devoted to the design of polymer acceptors as potential replacement for fullerene derivatives for high-performance all polymer solar cells (all-PSCs). One key factor that is limiting the efficiency of all-PSCs is the low fill factor (FF) (normally <0.65), which is strongly correlated with the mobility and film morphology of polymer:polymer blends. In this work, we find a facile method to modulate the crystallinity of the well-known naphthalene diimide (NDI) based polymer N2200, by replacing a certain amount of bithiophene (2T) units in the N2200 backbone by single thiophene (T) units and synthesizing a series of random polymers PNDI-Tx, where x is the percentage of the single T. The acceptor PNDI-T10 is properly miscible with the low band gap donor polymer PTB7-Th, and the nanostructured blend promotes efficient exciton dissociation and charge transport. Solvent annealing (SA) enables higher hole and electron mobilities, and further suppresses the bimolecular recombination. As expected, the PTB7-Th:PNDI-T10 solar cells attain a high PCE of 7.6%, which is a 2-fold increase compared to that of PTB7-Th:N2200 solar cells. The FF of 0.71 reaches the highest value among all-PSCs to date. Our work demonstrates a rational design for fine-tuned crystallinity of polymer acceptors, and reveals the high potential of all-PSCs through structure and morphology engineering of semicrystalline polymer:polymer blends.

14.
Beilstein J Org Chem ; 12: 1629-37, 2016.
Artigo em Inglês | MEDLINE | ID: mdl-27559416

RESUMO

Two high bandgap benzodithiophene-benzotriazole-based polymers were synthesized via palladium-catalysed Stille coupling reaction. In order to compare the effect of the side chains on the opto-electronic and photovoltaic properties of the resulting polymers, the benzodithiophene monomers were substituted with either octylthienyl (PTzBDT-1) or dihexylthienyl (PTzBDT-2) as side groups, while the benzotriazole unit was maintained unaltered. The optical characterization, both in solution and thin-film, indicated that PTzBDT-1 has a red-shifted optical absorption compared to PTzBDT-2, likely due to a more planar conformation of the polymer backbone promoted by the lower content of alkyl side chains. The different aggregation in the solid state also affects the energetic properties of the polymers, resulting in a lower highest occupied molecular orbital (HOMO) for PTzBDT-1 with respect to PTzBDT-2. However, an unexpected behaviour is observed when the two polymers are used as a donor material, in combination with PC61BM as acceptor, in bulk heterojunction solar cells. Even though PTzBDT-1 showed favourable optical and electrochemical properties, the devices based on this polymer present a power conversion efficiency of 3.3%, considerably lower than the efficiency of 4.7% obtained for the analogous solar cells based on PTzBDT-2. The lower performance is presumably attributed to the limited solubility of the PTzBDT-1 in organic solvents resulting in enhanced aggregation and poor intermixing with the acceptor material in the active layer.

15.
Phys Chem Chem Phys ; 18(16): 11132-8, 2016 Apr 28.
Artigo em Inglês | MEDLINE | ID: mdl-27051887

RESUMO

We have studied the photo-degradation in air of a blend of [6,6]-phenyl-C61-butyric acid methyl ester (PCBM) and poly[2,3-bis-(3-octyloxyphenyl)quinoxaline-5,8-diyl-alt-thiophene-2,5-diyl] (TQ1), and how the photo-degradation affects the solar cell performance. Using near-edge X-ray absorption fine structure (NEXAFS) spectroscopy, changes to the electronic structure of TQ1 and PCBM caused by illumination in ambient air are investigated and compared between the pristine materials and the blend. The NEXAFS spectra show that the unoccupied molecular orbitals of TQ1 are not significantly changed by the exposure of pristine TQ1 to light in air, whereas those of PCBM are severely affected as a result of photo-induced degradation of PCBM. Furthermore, the photo-degradation of PCBM is accelerated by blending it with TQ1. While the NEXAFS spectrum of TQ1 remains unchanged upon illumination in air, its valence band spectrum shows that the occupied molecular orbitals are weakly affected. Yet, UV-Vis absorption spectra demonstrate photo-bleaching of TQ1, which is attenuated in the presence of PCBM in blend films. Illumination of the active layer of TQ1:PCBM solar cells prior to cathode deposition causes severe losses in electrical performance.

16.
ACS Appl Mater Interfaces ; 7(49): 27106-14, 2015 Dec 16.
Artigo em Inglês | MEDLINE | ID: mdl-26592898

RESUMO

Two series of oligomers TQ and rhodanine end-capped TQ-DR were synthesized using a facile one-step method. Their optical, electrical, and thermal properties and photovoltaic performances were systematically investigated and compared. The TQ series of oligomers were found to be amorphous, whereas the TQ-DR series are semicrystalline. For the TQ oligomers, the results obtained in solar cells show that as the chain length of the oligomers increases, an increase in power conversion efficiency (PCE) is obtained. However, when introducing 3-ethylrhodanine into the TQ oligomers as end groups, the PCE of the TQ-DR series of oligomers decreases as the chain length increases. Moreover, the TQ-DR series of oligomers give much higher performances compared to the original amorphous TQ series of oligomers owing to the improved extinction coefficient (ε) and crystallinity afforded by the rhodanine. In particular, the highly crystalline oligomer TQ5-DR, which has the shortest conjugation length shows a high hole mobility of 0.034 cm(2) V(-1) s(-1) and a high PCE of 3.14%, which is the highest efficiency out of all of the six oligomers. The structure-property correlations for all of the oligomers and the TQ1 polymer demonstrate that structural control of enhanced intermolecular interactions and crystallinity is a key for small molecules/oligomers to achieve high mobilities, which is an essential requirement for use in OPVs.

17.
Phys Chem Chem Phys ; 17(40): 26677-89, 2015 Oct 28.
Artigo em Inglês | MEDLINE | ID: mdl-26394002

RESUMO

The spectral coverage of a light-harvesting polymer largely determines the maximum achievable photocurrent in organic photovoltaics, and therefore constitutes a crucial parameter for improving their performance. The D-A1-D-A2 copolymer motif is a new and promising design strategy for extending the absorption range by incorporating two acceptor units with complementary photoresponses. The fundamental factors that promote an extended absorption are here determined for three prototype D-A1-D-A2 systems through a combination of experimental and computational methods. Systematic quantum chemical calculations are then used to reveal the intrinsic optical properties of ten further D-A1-D-A2 polymer candidates. These investigated polymers are all predicted to exhibit intense primary absorption peaks at 615-954 nm, corresponding to charge-transfer (CT) transitions to the stronger acceptor, as well as secondary absorption features at 444-647 nm that originate from CT transitions to the weaker acceptors. Realization of D-A1-D-A2 polymers with superior spectral coverage is thereby found to depend critically on the spatial and energetic separation between the two distinct acceptor LUMOs. Two promising D-A1-D-A2 copolymer candidates were finally selected for further theoretical and experimental study, and demonstrate superior light-harvesting properties in terms of significantly extended spectral coverage. This demonstrates great potential for enhanced light-harvesting in D-A1-D-A2 polymers via multiple absorption features compared to traditional D-A polymers.

18.
Nanoscale ; 7(18): 8451-6, 2015 May 14.
Artigo em Inglês | MEDLINE | ID: mdl-25891364

RESUMO

The formation of fullerene crystals represents a major degradation pathway of polymer/fullerene bulk-heterojunction thin films that inexorably deteriorates their photovoltaic performance. Currently no tools exist that reveal the origin of fullerene crystal formation vertically through the film. Here, we show that electron tomography can be used to study nucleation and growth of fullerene crystals. A model bulk-heterojunction blend based on a thiophene-quinoxaline copolymer and a fullerene derivative is examined after controlled annealing above the glass transition temperature. We image a number of fullerene nanocrystals, ranging in size from 70 to 400 nanometers, and observe that their center is located close to the free-surface of spin-coated films. The results show that the nucleation of fullerene crystals predominately occurs in the upper part of the films. Moreover, electron tomography reveals that the nucleation is preceded by more pronounced phase separation of the blend components.

19.
Phys Chem Chem Phys ; 16(45): 24853-65, 2014 Dec 07.
Artigo em Inglês | MEDLINE | ID: mdl-25318819

RESUMO

A series of nine donor-acceptor polymers, including three new and six polymers from previous work, have been investigated experimentally and theoretically. The investigation focuses on narrow band gaps and strong absorptions of the polymers, where experimentally determined first peak absorption energies range from 1.8 to 2.3 eV, and peak absorption coefficients vary between 19-67 L g(-1) cm(-1). An overall assessment of each polymer's light-harvesting capability is made, and related to the chemical structure. Oligomer calculations using density functional theory are extrapolated to obtain size-converged polymer properties, and found to reproduce the experimental absorption trends well. Accurate theoretical predictions of absorption energies to within 0.06 eV of experiments, and absorption strength to within 12%, are obtained through the introduction of an empirical correction scheme. The computational and experimental results provide insight for the design of polymers with efficient absorption, concerning the intrinsic properties of the constituent units and the use of bulky side-groups.

20.
Adv Mater ; 26(12): 1801-26, 2014 Mar 26.
Artigo em Inglês | MEDLINE | ID: mdl-24523218

RESUMO

Driven by the potential advantages and promising applications of organic solar cells, donor-acceptor (D-A) polymers have been intensively investigated in the past years. One of the strong electron-withdrawing groups that were widely used as acceptors for the construction of D-A polymers for applications in polymer solar cells and FETs is isoindigo. The isoindigo-based polymer solar cells have reached efficiencies up to ∼7% and hole mobilities as high as 3.62 cm(2) V(-1) s(-1) have been realized by FETs based on isoindigo polymers. Over one hundred isoindigo-based small molecules and polymers have been developed in only three years. This review is an attempt to summarize the structures and properties of the isoindigo-based polymers and small molecules that have been reported in the literature since their inception in 2010. Focus has been given only to the syntheses and device performances of those polymers and small molecules that were designed for use in solar cells and FETs. Attempt has been made to deduce structure-property relationships that would guide the design of isoindigo-based materials. It is expected that this review will present useful guidelines for the design of efficient isoindigo-based materials for applications in solar cells and FETs.

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