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1.
Proc Natl Acad Sci U S A ; 118(38)2021 Sep 21.
Artigo em Inglês | MEDLINE | ID: mdl-34518214

RESUMO

Robust polymeric nanofilms can be used to construct gas-permeable soft electronics that can directly adhere to soft biological tissue for continuous, long-term biosignal monitoring. However, it is challenging to fabricate gas-permeable dry electrodes that can self-adhere to the human skin and retain their functionality for long-term (>1 d) health monitoring. We have succeeded in developing an extraordinarily robust, self-adhesive, gas-permeable nanofilm with a thickness of only 95 nm. It exhibits an extremely high skin adhesion energy per unit area of 159 µJ/cm2 The nanofilm can self-adhere to the human skin by van der Waals forces alone, for 1 wk, without any adhesive materials or tapes. The nanofilm is ultradurable, and it can support liquids that are 79,000 times heavier than its own weight with a tensile stress of 7.82 MPa. The advantageous features of its thinness, self-adhesiveness, and robustness enable a gas-permeable dry electrode comprising of a nanofilm and an Au layer, resulting in a continuous monitoring of electrocardiogram signals with a high signal-to-noise ratio (34 dB) for 1 wk.

2.
Nat Commun ; 12(1): 4937, 2021 Aug 16.
Artigo em Inglês | MEDLINE | ID: mdl-34400644

RESUMO

Solution processability of polymer semiconductors becomes an unfavorable factor during the fabrication of pixelated films since the underlying layer is vulnerable to subsequent solvent exposure. A foundry-compatible patterning process must meet requirements including high-throughput and high-resolution patternability, broad generality, ambient processability, environmentally benign solvents, and, minimal device performance degradation. However, known methodologies can only meet very few of these requirements. Here, a facile photolithographic approach is demonstrated for foundry-compatible high-resolution patterning of known p- and n-type semiconducting polymers. This process involves crosslinking a vertically phase-separated blend of the semiconducting polymer and a UV photocurable additive, and enables ambient processable photopatterning at resolutions as high as 0.5 µm in only three steps with environmentally benign solvents. The patterned semiconducting films can be integrated into thin-film transistors having excellent transport characteristics, low off-currents, and high thermal (up to 175 °C) and chemical (24 h immersion in chloroform) stability. Moreover, these patterned organic structures can also be integrated on 1.5 µm-thick parylene substrates to yield highly flexible (1 mm radius) and mechanically robust (5,000 bending cycles) thin-film transistors.

3.
Eur J Neurol ; 28(11): 3774-3783, 2021 11.
Artigo em Inglês | MEDLINE | ID: mdl-34255403

RESUMO

BACKGROUND AND PURPOSE: The purpose was to provide an overview of genotype and phenotype distribution in a cohort of patients with Charcot-Marie-Tooth disease (CMT) and related disorders from central south China. METHODS: In all, 435 patients were enrolled and detailed clinical data were collected. Multiplex ligation-dependent probe amplification for PMP22 duplication/deletion and CMT multi-gene panel sequencing were performed. Whole exome sequencing was further applied in the remaining patients who failed to achieve molecular diagnosis. RESULTS: Among the 435 patients, 216 had CMT1, 14 had hereditary neuropathy with pressure palsies (HNPP), 178 had CMT2, 24 had distal hereditary motor neuropathy (dHMN) and three had hereditary sensory and autonomic neuropathy (HSAN). The overall molecular diagnosis rate was 70%: 75.7% in CMT1, 100% in HNPP, 64.6% in CMT2, 41.7% in dHMN and 33.3% in HSAN. The most common four genotypes accounted for 68.9% of molecular diagnosed patients. Relatively frequent causes were missense changes in PMP22 (4.6%) and SH3TC2 (2.3%) in CMT1; and GDAP1 (5.1%), IGHMBP2 (4.5%) and MORC2 (3.9%) in CMT2. Twenty of 160 detected pathogenic variants and the associated phenotypes have not been previously reported. Broad phenotype spectra were observed in six genes, amongst which the pathogenic variants in BAG3 and SPTLC1 were detected in two sporadic patients presenting with the CMT2 phenotype. CONCLUSIONS: Our results provided a unique genotypic and phenotypic landscape of patients with CMT and related disorders from central south China, including a relatively high proportion of CMT2 and lower occurrence of PMP22 duplication. The broad phenotype spectra in certain genes have advanced our understanding of CMT.


Assuntos
Doença de Charcot-Marie-Tooth , Proteínas Adaptadoras de Transdução de Sinal , Proteínas Reguladoras de Apoptose , Doença de Charcot-Marie-Tooth/epidemiologia , Doença de Charcot-Marie-Tooth/genética , China/epidemiologia , Proteínas de Ligação a DNA , Genótipo , Humanos , Fenótipo , Fatores de Transcrição
5.
Proteomics ; 21(16): e2100035, 2021 08.
Artigo em Inglês | MEDLINE | ID: mdl-34132035

RESUMO

Arsenic pollution impacts health of millions of people in the world. Inorganic arsenic is a carcinogenic agent in skin and lung cancers. The stem-loop binding protein (SLBP) binds to the stem-loop of the canonical histone mRNA and regulates its metabolism during cell cycle. Our previous work has shown arsenic induces ubiquitin-proteasome dependent degradation of SLBP and contributes to lung cancer. In this study, we established the first comprehensive SLBP interaction network by affinity purification-mass spectrometry (AP-MS) analysis, and further demonstrated arsenic enhanced the association between SLBP and a crucial chaperone complex containing heat shock proteins (HSPs) and ERp44. Strikingly, knockdown of these proteins markedly rescued the protein level of SLBP under arsenic exposure conditions, and abolished the increasing migration capacity of BEAS-2B cells induced by arsenic. Taken together, our study provides a potential new mechanism that a chaperone complex containing HSPs and ERp44 attenuates the stability of SLBP under both normal and arsenic exposure conditions, which could be essential for arsenic-induced high cell migration.


Assuntos
Arsênio , Arsênio/toxicidade , Proteínas de Choque Térmico , Humanos , Proteínas de Membrana , Chaperonas Moleculares , Proteínas Nucleares/metabolismo , Ligação Proteica , Estabilidade Proteica , Proteômica , Fatores de Poliadenilação e Clivagem de mRNA
6.
Phys Chem Chem Phys ; 23(21): 12439-12448, 2021 Jun 02.
Artigo em Inglês | MEDLINE | ID: mdl-34031670

RESUMO

In recent years, two-dimensional (2D) lead-free double perovskites have been attracting much attention because of their unique performance in photovoltaic solar cells and photocatalysis. Nonetheless, how thickness affects the photoelectric properties of lead-free double perovskite remains unclear. In this work, by means of density functional theory (DFT) with a spin orbit coupling (SOC) effect, we have investigated the electronic and optical properties systemically, including band structures, carrier mobility, optical absorption spectra, exciton-binding energies, band edges alignment and molecule adsorption performance of Cs2AgBiBr6 with different thicknesses. The calculated results revealed the thickness-induced band gap and optical performance for Cs2AgBiBr6. It shows a low band gap and outstanding optical absorption of visible and ultraviolet light. When the thickness is reduced to a monolayer, Cs2AgBiBr6 moves from an indirect band gap to a direct band gap. Moreover, the carrier mobility of Cs2AgBiBr6 is excellent and the exciton-binding energy increases with the decreased thickness. Importantly, an analysis of molecule adsorption and band edge alignment indicates that Cs2AgBiBr6 is prone to H2O adsorption and H2 desorption theoretically, which is conducive to the photocatalytic water splitting for hydrogen generation and other photovatalytic reactions. Our work suggests that Cs2AgBiBr6 is a potential candidate as a solar cell or a photocatalyst, and we provide theoretical explorations into reducing the layers of lead-free double perovskite materials to 2D atomic thickness for a better photocatalytic application, which can serve as guidelines for the design of excellent photocatalysts.

7.
Front Bioeng Biotechnol ; 9: 641130, 2021.
Artigo em Inglês | MEDLINE | ID: mdl-33842445

RESUMO

Design an implant similar to the human bone is one of the critical problems in bone tissue engineering. Metal porous scaffolds have good prospects in bone tissue replacement due to their matching elastic modulus, better strength, and biocompatibility. However, traditional processing methods are challenging to fabricate scaffolds with a porous structure, limiting the development of porous scaffolds. With the advancement of additive manufacturing (AM) and computer-aided technologies, the development of porous metal scaffolds also ushers in unprecedented opportunities. In recent years, many new metal materials and innovative design methods are used to fabricate porous scaffolds with excellent mechanical properties and biocompatibility. This article reviews the research progress of porous metal scaffolds, and introduces the AM technologies used in porous metal scaffolds. Then the applications of different metal materials in bone scaffolds are summarized, and the advantages and limitations of various scaffold design methods are discussed. Finally, we look forward to the development prospects of AM in porous metal scaffolds.

8.
Adv Mater ; 33(14): e2007041, 2021 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-33655643

RESUMO

Organic polymer electrochemical transistors (OECTs) are of great interest for flexible electronics and bioelectronics applications owing to their high transconductance and low operating voltage. However, efficient OECT operation must delicately balance the seemingly incompatible materials optimizations of redox chemistry, active layer electronic transport, and ion penetration/transport. The latter characteristics are particularly challenging since most high-mobility semiconducting polymers are hydrophobic, which hinders efficient ion penetration, hence limiting OECT performance. Here, the properties and OECT response of a series of dense and porous semiconducting polymer films are compared, the latter fabricated via a facile breath figure approach. This methodology enables fast ion doping, high transconductance (up to 364 S cm-1 ), and a low subthreshold swing for the hydrophobic polymers DPPDTT and P3HT, rivalling or exceeding the metrics of the relatively hydrophilic polymer, Pg2T-T. Furthermore, the porous morphology also enhances the transconductance of hydrophilic polymers, offering a general strategy for fabricating high-performance electrochemical transistors.

9.
ACS Appl Mater Interfaces ; 13(13): 15399-15408, 2021 Apr 07.
Artigo em Inglês | MEDLINE | ID: mdl-33779161

RESUMO

Metal oxide semiconductors, such as amorphous indium gallium zinc oxide (a-IGZO), have made impressive strides as alternatives to amorphous silicon for electronics applications. However, to achieve the full potential of these semiconductors, compatible unconventional gate dielectric materials must also be developed. To this end, solution-processable self-assembled nanodielectrics (SANDs) composed of structurally well-defined and durable nanoscopic alternating organic (e.g., stilbazolium) and inorganic oxide (e.g., ZrOx and HfOx) layers offer impressive capacitances and low processing temperatures (T ≤ 200 °C). While SANDs have been paired with diverse semiconductors and have yielded excellent device metrics, they have never been implemented in the most technologically relevant top-gate thin-film transistor (TFT) architecture. Here, we combine solution-processed a-IGZO with solution-processed four-layer Hf-SAND to fabricate top-gate TFTs, which exhibit impressive electron mobilities (µSAT = 19.4 cm2 V-1 s-1) and low threshold voltages (Vth = 0.83 V), subthreshold slopes (SS = 293 mV/dec), and gate leakage currents (10-10 A) as well as high bias stress stability.

10.
ACS Appl Mater Interfaces ; 13(2): 3445-3453, 2021 Jan 20.
Artigo em Inglês | MEDLINE | ID: mdl-33416304

RESUMO

Low-temperature, solution-processable, high-capacitance, and low-leakage gate dielectrics are of great interest for unconventional electronics. Here, we report a near room temperature ultraviolet densification (UVD) methodology for realizing high-performance organic-inorganic zirconia self-assembled nanodielectrics (UVD-ZrSANDs). These UVD-ZrSAND multilayers are grown from solution in ambient, densified by UV radiation, and characterized by X-ray reflectivity, atomic force microscopy, X-ray photoelectron spectroscopy, and capacitance measurements. The resulting UVD-ZrSAND films exhibit large capacitances of >700 nF/cm2 and low leakage current densities of <10-7 A/cm2, which rival or exceed those synthesized by traditional thermal methods. Both the p-type organic semiconductor pentacene and the n-type metal oxide semiconductor In2O3 were used to investigate UVD-ZrSANDs as the gate dielectric in thin-film transistors, affording mobilities of 0.58 and 26.21 cm2/(V s), respectively, at a low gate voltage of 2 V. These results represent a significant advance in fabricating ultra-thin high-performance dielectrics near room temperature and should facilitate their integration into diverse electronic technologies.

11.
Angew Chem Int Ed Engl ; 60(3): 1433-1440, 2021 Jan 18.
Artigo em Inglês | MEDLINE | ID: mdl-33006403

RESUMO

The introduction of oxygen vacancies (Ov) has been regarded as an effective method to enhance the catalytic performance of photoanodes in oxygen evolution reaction (OER). However, their stability under highly oxidizing environment is questionable but was rarely studied. Herein, NiFe-metal-organic framework (NiFe-MOFs) was conformally coated on oxygen-vacancy-rich BiVO4 (Ov-BiVO4 ) as the protective layer and cocatalyst, forming a core-shell structure with caffeic acid as bridging agent. The as-synthesized Ov-BiVO4 @NiFe-MOFs exhibits enhanced stability and a remarkable photocurrent density of 5.3±0.15 mA cm-2 at 1.23 V (vs. RHE). The reduced coordination number of Ni(Fe)-O and elevated valence state of Ni(Fe) in NiFe-MOFs layer greatly bolster OER, and the shifting of oxygen evolution sites from Ov-BiVO4 to NiFe-MOFs promotes Ov stabilization. Ovs can be effectively preserved by the coating of a thin NiFe-MOFs layer, leading to a photoanode of enhanced photocurrent and stability.

12.
Front Neurol ; 11: 603003, 2020.
Artigo em Inglês | MEDLINE | ID: mdl-33381078

RESUMO

Background and Objectives: Distal hereditary motor neuropathy (dHMN) is a clinically and genetically heterogeneous group of inherited neuropathies. The objectives of this study were to report the clinical and genetic features of dHMN patients in a Chinese cohort. Aims and Methods: We performed clinical assessments and whole-exome sequencing in 24 dHMN families from Mainland China. We conducted a retrospective analysis of the data and investigated the frequency and clinical features of patients with a confirmed mutation. Results: Two novel heterozygous mutations in GARS, c.373G>C (p.E125Q) and c.1015G>A (p.G339R), were identified and corresponded to the typical dHMN-V phenotype. Together with families with WARS, SORD, SIGMAR1, and HSPB1 mutations, 29.2% of families (7/24) acquired a definite genetic diagnosis. One novel heterozygous variant of uncertain significance, c.1834G>A (p.G612S) in LRSAM1, was identified in a patient with mild dHMN phenotype. Conclusion: Our study expanded the mutation spectrum of GARS mutations and added evidence that GARS mutations are associated with both axonal Charcot-Marie-Tooth and dHMN phenotypes. Mutations in genes encoding aminoamide tRNA synthetase (ARS) might be a frequent cause of autosomal dominant-dHMN, and SORD mutation might account for a majority of autosomal recessive-dHMN cases. The relatively low genetic diagnosis yield indicated more causative dHMN genes need to be discovered.

13.
Angew Chem Int Ed Engl ; 59(46): 20522-20528, 2020 Nov 09.
Artigo em Inglês | MEDLINE | ID: mdl-32717146

RESUMO

Polar functionalized isotactic and syndiotactic polypropylenes (PPs) are synthesized by direct, masking-reagent-free propylene and amino-olefin (AO, CH2 =CH(CH2 )x Nn Pr2 , x=2, 3, 6) copolymerizations using the activated precatalysts rac-[Me2 Si(indenyl)2 ]ZrMe2 and [Me2 C(Cp)(fluorenyl)]ZrMe2 , respectively. Polymerization activities at 25 °C are as high as 4208 and 535 kg/(mol h atm) with AO incorporation up to 4.0 mol % and 1.6 mol %, respectively. Remarkably, introducing the amino-olefin comonomers significantly enhances stereoselection for both isotactic (mmmm: 59.5 %→91.0 %) and syndiotactic (rrrr: 66.3 %→81.3 %) products.

14.
Proc Natl Acad Sci U S A ; 117(31): 18231-18239, 2020 Aug 04.
Artigo em Inglês | MEDLINE | ID: mdl-32703807

RESUMO

The field-effect electron mobility of aqueous solution-processed indium gallium oxide (IGO) thin-film transistors (TFTs) is significantly enhanced by polyvinyl alcohol (PVA) addition to the precursor solution, a >70-fold increase to 7.9 cm2/Vs. To understand the origin of this remarkable phenomenon, microstructure, electronic structure, and charge transport of IGO:PVA film are investigated by a battery of experimental and theoretical techniques, including In K-edge and Ga K-edge extended X-ray absorption fine structure (EXAFS); resonant soft X-ray scattering (R-SoXS); ultraviolet photoelectron spectroscopy (UPS); Fourier transform-infrared (FT-IR) spectroscopy; time-of-flight secondary-ion mass spectrometry (ToF-SIMS); composition-/processing-dependent TFT properties; high-resolution solid-state 1H, 71Ga, and 115In NMR spectroscopy; and discrete Fourier transform (DFT) analysis with ab initio molecular dynamics (MD) liquid-quench simulations. The 71Ga{1H} rotational-echo double-resonance (REDOR) NMR and other data indicate that PVA achieves optimal H doping with a Ga···H distance of ∼3.4 Å and conversion from six- to four-coordinate Ga, which together suppress deep trap defect localization. This reduces metal-oxide polyhedral distortion, thereby increasing the electron mobility. Hydroxyl polymer doping thus offers a pathway for efficient H doping in green solvent-processed metal oxide films and the promise of high-performance, ultra-stable metal oxide semiconductor electronics with simple binary compositions.

15.
ACS Appl Mater Interfaces ; 12(31): 34901-34909, 2020 Aug 05.
Artigo em Inglês | MEDLINE | ID: mdl-32633937

RESUMO

Self-assembled nanodielectrics (SANDs) consist of alternating layers of polarized phosphonate-functionalized azastibazolium π-electron (PAE) and high-k dielectric metal oxide (ZrO2 or HfOx) films. SANDs are desirable gate dielectrics materials for thin-film transistor applications because of their excellent properties such as low-temperature fabrication, large dielectric strength, and large capacitance. In this paper, we investigate the cross-plane thermal boundary conductance of SANDs using the frequency domain thermoreflectance (FDTR) technique. First, we characterize the thermal conductance of PAE self-assembled monolayers (SAMs), inverted-PAE (IPAE) SAMs, and mixed PAE-IPAE SAMs, sandwiched between thin gold and silica (SiO2) films at the top and bottom surfaces. Next, we quantify the thermal conductance of SAND-n with different numbers (n) of PAE-ZrO2 layers and thicknesses ranging between 4.7 and 11.3 nm. From the FDTR measurements, we observe that the thermal boundary conductance of the SAMs can be tuned between 42.1 ± 4.6 MW/(m2 K) and 52.4 ± 2.5 MW/(m2 K), based on the relative density of the PAE and IPAE chromophores. In the SAND-n samples, we observe a monotonic decrease in the thermal conductance with increasing n. We use the measured thermal conductance data in a series resistance model to estimate a thermal interface conductance of 695 MW/(m2 K) for the contact between the PAE chromophore and the zirconium dioxide films, which is an order of magnitude larger than the SAMs. We attribute the improved thermal conductance to stronger adhesion between the PAE chromophore and the zirconium dioxide films, as compared to the weakly bonded SAMs to the gold and silicon dioxide films.

16.
Proc Natl Acad Sci U S A ; 117(30): 17551-17557, 2020 Jul 28.
Artigo em Inglês | MEDLINE | ID: mdl-32647062

RESUMO

The rational creation of two-component conjugated polymer systems with high levels of phase purity in each component is challenging but crucial for realizing printed soft-matter electronics. Here, we report a mixed-flow microfluidic printing (MFMP) approach for two-component π-polymer systems that significantly elevates phase purity in bulk-heterojunction solar cells and thin-film transistors. MFMP integrates laminar and extensional flows using a specially microstructured shear blade, designed with fluid flow simulation tools to tune the flow patterns and induce shear, stretch, and pushout effects. This optimizes polymer conformation and semiconducting blend order as assessed by atomic force microscopy (AFM), transmission electron microscopy (TEM), grazing incidence wide-angle X-ray scattering (GIWAXS), resonant soft X-ray scattering (R-SoXS), photovoltaic response, and field effect mobility. For printed all-polymer (poly[(5,6-difluoro-2-octyl-2H-benzotriazole-4,7-diyl)-2,5-thiophenediyl[4,8-bis[5-(2-hexyldecyl)-2-thienyl]benzo[1,2-b:4,5-b']dithiophene-2,6-diyl]-2,5-thiophenediyl]) [J51]:(poly{[N,N'-bis(2-octyldodecyl)naphthalene-1,4,5,8-bis(dicarboximide)-2,6-diyl]-alt-5,5'-(2,2'-bithiophene)}) [N2200]) solar cells, this approach enhances short-circuit currents and fill factors, with power conversion efficiency increasing from 5.20% for conventional blade coating to 7.80% for MFMP. Moreover, the performance of mixed polymer ambipolar [poly(3-hexylthiophene-2,5-diyl) (P3HT):N2200] and semiconducting:insulating polymer unipolar (N2200:polystyrene) transistors is similarly enhanced, underscoring versatility for two-component π-polymer systems. Mixed-flow designs offer modalities for achieving high-performance organic optoelectronics via innovative printing methodologies.

17.
J Am Chem Soc ; 142(28): 12440-12452, 2020 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-32539371

RESUMO

The frequency-dependent capacitance of low-temperature solution-processed metal oxide (MO) dielectrics typically yields unreliable and unstable thin-film transistor (TFT) performance metrics, which hinders the development of next-generation roll-to-roll MO electronics and obscures intercomparisons between processing methodologies. Here, capacitance values stable over a wide frequency range are achieved in low-temperature combustion-synthesized aluminum oxide (AlOx) dielectric films by fluoride doping. For an optimal F incorporation of ∼3.7 atomic % F, the F:AlOx film capacitance of 166 ± 11 nF/cm2 is stable over a 10-1-104 Hz frequency range, far more stable than that of neat AlOx films (capacitance = 336 ± 201 nF/cm2) which falls from 781 ± 85 nF/cm2 to 104 ± 4 nF/cm2 over this frequency range. Importantly, both n-type/inorganic and p-type/organic TFTs exhibit reliable electrical characteristics with minimum hysteresis when employing the F:AlOx dielectric with ∼3.7 atomic % F. Systematic characterization of film microstructural/compositional and electronic/dielectric properties by X-ray photoelectron spectroscopy, time-of-fight secondary ion mass spectrometry, cross-section transmission electron microscopy, solid-state nuclear magnetic resonance, and UV-vis absorption spectroscopy reveal that fluoride doping generates AlOF, which strongly reduces the mobile hydrogen content, suppressing polarization mechanisms at low frequencies. Thus, this work provides a broadly applicable anion doping strategy for the realization of high-performance solution-processed metal oxide dielectrics for both organic and inorganic electronics applications.

18.
Nat Commun ; 11(1): 2405, 2020 05 15.
Artigo em Inglês | MEDLINE | ID: mdl-32415064

RESUMO

Fiber-based electronics enabling lightweight and mechanically flexible/stretchable functions are desirable for numerous e-textile/e-skin optoelectronic applications. These wearable devices require low-cost manufacturing, high reliability, multifunctionality and long-term stability. Here, we report the preparation of representative classes of 3D-inorganic nanofiber network (FN) films by a blow-spinning technique, including semiconducting indium-gallium-zinc oxide (IGZO) and copper oxide, as well as conducting indium-tin oxide and copper metal. Specifically, thin-film transistors based on IGZO FN exhibit negligible performance degradation after one thousand bending cycles and exceptional room-temperature gas sensing performance. Owing to their great stretchability, these metal oxide FNs can be laminated/embedded on/into elastomers, yielding multifunctional single-sensing resistors as well as fully monolithically integrated e-skin devices. These can detect and differentiate multiple stimuli including analytes, light, strain, pressure, temperature, humidity, body movement, and respiratory functions. All of these FN-based devices exhibit excellent sensitivity, response time, and detection limits, making them promising candidates for versatile wearable electronics.


Assuntos
Nanopartículas Metálicas/química , Nanofibras/química , Dispositivos Eletrônicos Vestíveis , Consumo de Bebidas Alcoólicas , Técnicas Biossensoriais , Testes Respiratórios , Cobre/química , Elastômeros , Etanol/análise , Análise de Elementos Finitos , Gálio/química , Humanos , Índio/química , Teste de Materiais , Movimento (Física) , Poliestirenos/química , Semicondutores , Espectrofotometria Ultravioleta , Temperatura , Têxteis , Óxido de Zinco/química
19.
Sci Adv ; 6(13): eaaz1042, 2020 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-32232157

RESUMO

Porous semiconductor film morphologies facilitate fluid diffusion and mass transport into the charge-carrying layers of diverse electronic devices. Here, we report the nature-inspired fabrication of several porous organic semiconductor-insulator blend films [semiconductor: P3HT (p-type polymer), C8BTBT (p-type small-molecule), and N2200 (n-type polymer); insulator: PS] by a breath figure patterning method and their broad and general applicability in organic thin-film transistors (OTFTs), gas sensors, organic electrochemical transistors (OECTs), and chemically doped conducting films. Detailed morphological analysis of these films demonstrates formation of textured layers with uniform nanopores reaching the bottom substrate with an unchanged solid-state packing structure. Device data gathered with both porous and dense control semiconductor films demonstrate that the former films are efficient TFT semiconductors but with added advantage of enhanced sensitivity to gases (e.g., 48.2%/ppm for NO2 using P3HT/PS), faster switching speeds (4.7 s for P3HT/PS OECTs), and more efficient molecular doping (conductivity, 0.13 S/m for N2200/PS).

20.
J Am Chem Soc ; 142(12): 5487-5492, 2020 Mar 25.
Artigo em Inglês | MEDLINE | ID: mdl-32053356

RESUMO

Mechanically flexible films of the highly crystalline core-cyanated perylenediimide (PDIF-CN2) molecular semiconductor are achieved via a novel grain boundary plasticization strategy in which a specially designed polymeric binder (PB) is used to connect crystallites at the grain boundaries. The new PB has a naphthalenediimide-dithiophene π-conjugated backbone end-functionalized with PDI units. In contrast to conventional polymer-small molecule blends where distinct phase separation occurs, this blend film with plasticized grain boundaries exhibits a morphology typical of homogeneous PDIF-CN2 films which is preserved upon bending at radii as small as 2 mm. Thin-film transistors fabricated with PB/PDIF-CN2 blends exhibit substantial electron mobilities even after repeated bending. This design represents a new approach to realizing flexible and textured semiconducting π-electron films with good mechanical and charge transport properties.

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