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1.
ChemSusChem ; : e202400636, 2024 Jun 03.
Artigo em Inglês | MEDLINE | ID: mdl-38828662

RESUMO

The stability of high-energy-density lithium metal batteries (LMBs) heavily relies on the composition of the solid electrolyte interphase (SEI) formed on lithium metal anodes. In this study, the inorganic-rich SEI layer was achieved by incorporating bisalts additives into carbonate-based electrolytes. Within this SEI layer, the presence of LiF, polythionate, and Li3N was observed, generated by combining 1.0 м lithium bis(trifluoromethanesulfonyl)imide in ethylene carbonate: ethyl methyl carbonate:dimethyl carbonate in a 1:1:1 volume ratio, with the addition of 2 wt% lithium difluorophosphate and 2 wt% lithium difluoro(oxalato)borate additives (EL-DO). Furthermore, this formulation effectively mitigated corrosion of aluminum current collectors. EL-DO exhibited outstanding performance, including an average coulombic efficiency of 98.2% in Li||Cu cells and a stable discharge capacity of approximately 162 mAh g-1 after 200 cycles in a Li||LiNi0.8Co0.1Mn0.1O2 (NCM811) configuration. Moreover, EL-DO displayed the potential to enhance the performance not only of LMBs but also of lithium-ion batteries. In the case of Gr||NCM811 cell using EL-DO, it consistently maintained high discharge capacities, even achieving around 135 mAh g-1 after the 100th cycle, surpassing the performance of other electrolytes. This study underscores the synergistic impact of bisalts additives in elevating the performance of lithium batteries.

2.
ACS Nano ; 18(14): 10156-10164, 2024 Apr 09.
Artigo em Inglês | MEDLINE | ID: mdl-38551612

RESUMO

Curvature is a general factor for various two-dimensional (2D) materials due to their flexibility, which is not yet fully unveiled to control their physical properties. In particular, the effect of structural disorder with random curvature formation on excitons in 2D semiconductors is not fully understood. Here, the correlation between structural disorder and exciton formation in monolayer MoS2 on SiO2 was investigated by using photoluminescence (PL) and Raman spectroscopy. We found that the curvature-induced charge localization along with band gap fluctuations aid the formation of the localized charged excitons (such as trions). In the substrate-supported region, the trion population is enhanced by a localized charge due to the microscopic random bending strain, while the trion is suppressed in the suspended region which exhibits negligible bending strain, anomalously even though the dielectric screening effect is lower than that of the supported region. The redistribution of each exciton by the bending strain leads to a huge variation (∼100-fold) in PL intensity between the supported and suspended regions, which cannot be fully comprehended by external potential disorders such as a random distribution of charged impurities. The peak position of PL in MoS2/SiO2 is inversely proportional to the Raman peak position of E12g, indicating that the bending strain is correlated with PL. The supported regions exhibit an indirect portion that was not shown in the suspended regions or atomically flat substrates. The understanding of the structural disorder effect on excitons provides a fundamental path for optoelectronics and strain engineering of 2D semiconductors.

3.
ACS Nano ; 18(5): 4432-4442, 2024 Feb 06.
Artigo em Inglês | MEDLINE | ID: mdl-38284564

RESUMO

Two-dimensional transition-metal dichalcogenides have attracted significant attention because of their unique intrinsic properties, such as high transparency, good flexibility, atomically thin structure, and predictable electron transport. However, the current state of device performance in monolayer transition-metal dichalcogenide-based optoelectronics is far from commercialization, because of its substantial strain on the heterogeneous planar substrate and its robust metal deposition, which causes crystalline damage. In this study, we show that strain-relaxed and undamaged monolayer WSe2 can improve a device performance significantly. We propose here an original point-cell-type photodetector. The device consists in a monolayer of an absorbing TMD (i.e., WSe2) simply deposited on a structured electrode, i.e., core-shell silicon-gold nanopillars. The maximum photoresponsivity of the device is found to be 23.16 A/W, which is a significantly high value for monolayer WSe2-based photodetectors. Such point-cell photodetectors can resolve the critical issues of 2D materials, leading to tremendous improvements in device performance.

4.
ACS Appl Mater Interfaces ; 16(6): 8016-8023, 2024 Feb 14.
Artigo em Inglês | MEDLINE | ID: mdl-38294420

RESUMO

The photoelectrochemical water splitting (PEC-WS) performance of a photoanode consisting of GaN nanowires (NWs) is significantly improved using a Ti3C2-MXene coating as an intermediate layer to promote carrier transfer toward the electrolyte. The maximum current density and applied-bias photon-to-current efficiency of the photoanode comprising GaN NWs coated with Ti3C2-MXene (MGNWs) are measured to be 34.24 mA/cm2 and 14.47% at 1.2 and 0.4 V versus a reversible hydrogen electrode (RHE), respectively. These values are much higher than those of the GaN-NW photoanode without Ti3C2-MXene (4.04 mA/cm2 and 1.95%) and also markedly exceed those of previously reported photoanodes. After 8 days of PEC-WS, the current density was measured to be 31.07 mA/cm2, which corresponds to 97.58% of that measured immediately after the reaction started. Based on the time dependence of the current density, the hydrogen evolution rate over the reaction time is calculated to be 0.58 mmol/cm2·h. The results confirm that the PEC-WS performance of the optimized MGNW photoanode is superior to and more stable than those of previously reported photoanodes.

5.
Nanomaterials (Basel) ; 14(2)2024 Jan 19.
Artigo em Inglês | MEDLINE | ID: mdl-38276732

RESUMO

Perovskite solar cells (PSCs) have been significantly improved by utilizing an inorganic hole-transporting layer (HTL), such as nickel oxide. Despite the promising properties, there are still limitations due to defects. Recently, research on self-assembled monolayers (SAMs) is being actively conducted, which shows promise in reducing defects and enhancing device performance. In this study, we successfully engineered a p-i-n perovskite solar cell structure utilizing HC-A1 and HC-A4 molecules. These SAM molecules were found to enhance the grain morphology and uniformity of the perovskite film, which are critical factors in determining optical properties and device performance. Notably, HC-A4 demonstrated superior performance due to its distinct hydrophilic properties with a contact angle of 50.3°, attributable to its unique functional groups. Overall, the HC-A4-applied film exhibited efficient carrier extraction properties, attaining a carrier lifetime of 117.33 ns. Furthermore, HC-A4 contributed to superior device performance, achieving the highest device efficiency of 20% and demonstrating outstanding thermal stability over 300 h.

6.
Small ; 18(14): e2107492, 2022 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-35212457

RESUMO

Li metal batteries (LMBs) are ideal candidates for future high-energy-density battery systems. To date, high-voltage LMBs suffer severe limitations because of electrolytes unstable against Li anodes and high-voltage cathodes. Although ether-based electrolytes exhibit good stability with Li metal, compared to carbonate-based electrolytes, they have been used only in ≤4.0 V LMBs because of their limited oxidation stability. Here, a high concentration electrolyte (HCE) comprising lithium bis(fluorosulfonyl)imide (LiFSI) and a weakly solvating solvent (1,2-diethoxyethane, DEE) is designed, which can regulate unique solvation structures with only associated complexes at relatively lower concentration compared to the reported HCEs. This effectively suppresses dendrites on the anode side, and preserves the structural integrity of the cathode side under high voltages by the formation of stable interfacial layers on a Li metal anode and LiNi0.8 Mn0.1 Co0.1 O2 (NMC811) cathode. Consequently, a 3.5 m LiFSI-DEE plays an important role in enhancing the stability of the Li||NMC811 cell with a capacity retention of ≈94% after 200 cycles under a high current density of 2.5 mA cm-2 . In addition, the 3.5 m LiFSI-DEE electrolyte exhibits good performance with anode-free batteries. This study offers a promising approach to enable ether-based electrolytes for high-voltage LMBs applications.

7.
ACS Appl Mater Interfaces ; 13(46): 55489-55497, 2021 Nov 24.
Artigo em Inglês | MEDLINE | ID: mdl-34761893

RESUMO

The instability of van der Waals (vdW) materials leads to spontaneous morphological and chemical transformations in the air. Although the passivation of vdW materials with other resistive materials is often used to solve stability issues, this passivation layer can block carrier injection and thus interfere with charge transfer doping. In this study, a facile method is proposed for n-doping and mediation of Se vacancies in tungsten diselenide (WSe2) by poly(vinylpyrrolidone) (PVP) coating. The major carrier type of the PVP-coated WSe2-based field-effect transistor (FET) was converted from hole (p-type) to electron (n-type). Furthermore, the vacancy-induced interface trap density was reduced by approximately 500 times. This study provides a practical doping and passivation method for the van der Waals materials, as well as a comprehensive understanding of the chemical reaction and electronic transport in these materials.

8.
ACS Nano ; 14(9): 11985-11994, 2020 Sep 22.
Artigo em Inglês | MEDLINE | ID: mdl-32840363

RESUMO

Monolayer transition metal dichalcogenides (TMDs) with a direct band gap are suitable for various optoelectronic applications such as ultrathin light emitters and absorbers. However, their weak light absorption caused by the atomically thin layer hinders more versatile applications for high optical gains. Although plasmonic hybridization with metal nanostructures significantly enhances light-matter interactions, the corrosion, instability of the metal nanostructures, and the undesired effects of direct metal-semiconductor contact act as obstacles to its practical application. Herein, we propose a dielectric nanostructure for plasmon-enhanced light-matter interaction of TMDs. TiO2 nanowires (NWs), as an example, are hybridized with a MoS2 monolayer on various substrates. The structure is implemented by placing a monolayer MoS2 between a TiO2 NW for a photonic scattering effect and metallic substrates with a spacer for the plasmonic Purcell effect. Here, the thin dielectric spacer is aimed at minimizing emission quenching from direct metal contact, while maximizing optical field localization in ultrathin MoS2 near the TiO2 NW. An effective emission enhancement factor of ∼22 is attained for MoS2 near the NW of the hybrid structure compared to the one without NWs. Our work is expected to facilitate a hybridized platform based on 2D semiconductors for high-performance and robust optoelectronics via engineering dielectric nanostructures with plasmonic materials.

9.
Nano Lett ; 20(4): 2370-2377, 2020 Apr 08.
Artigo em Inglês | MEDLINE | ID: mdl-32031411

RESUMO

We study the electronic and optoelectronic properties of a broken-gap heterojunction composed of SnSe2 and MoTe2 with gate-controlled junction modes. Owing to the interband tunneling current, our device can act as an Esaki diode and a backward diode with a peak-to-valley current ratio approaching 5.7 at room temperature. Furthermore, under an 811 nm laser irradiation the heterostructure exhibits a photodetectivity of up to 7.5 × 1012 Jones. In addition, to harness the electrostatic gate bias, Voc can be tuned from negative to positive by switching from the accumulation mode to the depletion mode of the heterojunction. Additionally, a photovoltaic effect with a fill factor exceeding 41% was observed, which highlights the significant potential for optoelectronic applications. This study not only demonstrates high-performance multifunctional optoelectronics based on the SnSe2/MoTe2 heterostructure but also provides a comprehensive understanding of broken-band alignment and its applications.

10.
Sci Rep ; 9(1): 15461, 2019 Oct 29.
Artigo em Inglês | MEDLINE | ID: mdl-31664111

RESUMO

We demonstrated an effective poly(p-chloro-xylylene) (Parylene-C) encapsulation method for MAPbI3 solar cells. By structural and optical analysis, we confirmed that Parylene-C efficiently slowed the decomposition reaction in MAPbI3. From a water permeability test with different encapsulating materials, we found that Parylene-C-coated MAPbI3 perovskite was successfully passivated from reaction with water, owing to the hydrophobic behavior of Parylene-C. As a result, the Parylene-C-coated MAPbI3 solar cells showed better device stability than uncoated cells, virtually maintaining the initial power conversion efficiency value (15.5 ± 0.3%) for 196 h.

11.
Sci Rep ; 9(1): 5900, 2019 Apr 11.
Artigo em Inglês | MEDLINE | ID: mdl-30976032

RESUMO

We fabricated the stacked bilayer molybdenum disulfide (MoS2) by using reduced graphene oxide (rGO) as a spacer for increasing the optoelectronic properties of MoS2. The rGO can decrease the interlayer coupling between the stacked bilayer MoS2 and retain the direct band gap property of MoS2. We observed a twofold enhancement of the photoluminescence intensity of the stacked MoS2 bilayer. In the Raman scattering, we observed that the E12g and A1g modes of the stacked bilayer MoS2 with rGO were further shifted compared to monolayer MoS2, which is due to the van der Waals (vdW) interaction and the strain effect between the MoS2 and rGO layers. The findings of this study will expand the applicability of monolayer MoS2 for high-performance optoelectronic devices by enhancing the optical properties using a vdW spacer.

12.
Nanoscale ; 10(43): 20306-20312, 2018 Nov 08.
Artigo em Inglês | MEDLINE | ID: mdl-30375621

RESUMO

Two-dimensional transition-metal dichalcogenides (TMDCs) are notable materials owing to their flexibility, transparency, and appropriate bandgaps. Because of their unique advantages, TMDC p-n diodes have been studied for next-generation electronics and optoelectronics. However, their efficiency must be increased for commercialization. In this study, we demonstrated a heterostructure composed of few-layer ReS2 and WSe2. This few-layer ReS2/WSe2 heterostructure exhibits a p-n junction and an n-n junction in different gate-bias regimes. In the p-n junction regime, the heterostructure shows outstanding rectification behavior. Additionally, we identify three carrier-transfer mechanisms - direct tunneling, Fowler-Nordheim tunneling, and the space charge region - depending on the drain bias. Furthermore, the photovoltaic effect is observed in this few-layer ReS2/WSe2 heterostructure. As a result, a high fill factor (≈ 0.56), power conversion (≈ 1.5%), and external quantum efficiency (≈ 15.3%) were obtained. This study provides new guidelines for flexible optoelectronic devices.

13.
Biomater Res ; 22: 30, 2018.
Artigo em Inglês | MEDLINE | ID: mdl-30275973

RESUMO

BACKGROUND: Mucoadhesive polymers, which may increase the contact time between the polymer and the tissue, have been widely investigated for pharmaceutical formulations. In this study, we developed a new polysaccharide-based mucoadhesive polymer with thermogelling properties. METHODS: Hexanoyl glycol chitosan (HGC), a new thermogelling polymer, was synthesized by the chemical modification of glycol chitosan using hexanoic anhydride. The HGC was further modified to include thiol groups to improve the mucoadhesive property of thermogelling HGC. The degree of thiolation of the thiolated HGCs (SH-HGCs) was controlled in the range of 5-10% by adjusting the feed molar ratio. The structure of the chemically modified polymers was characterized by 1H NMR and ATR-FTIR. The sol-gel transition, mucoadhesiveness, and biocompatibility of the polymers were determined by a tube inverting method, rheological measurements, and in vitro cytotoxicity tests, respectively. RESULTS: The aqueous solution (4 wt%) of HGC with approximately 33% substitution showed a sol-gel transition temperature of approximately 41 °C. SH-HGCs demonstrated lower sol-gel transition temperatures (34 ± 1 and 31 ± 1 °Ð¡) compared to that of HGC due to the introduction of thiol groups. Rheological studies of aqueous mixture solutions of SH-HGCs and mucin showed that SH-HGCs had stronger mucoadhesiveness than HGC due to the interaction between the thiol groups of SH-HGCs and mucin. Additionally, we confirmed that the thermogelling properties might improve the mucoadhesive force of polymers. Several in vitro cytotoxicity tests showed that SH-HGCs showed little toxicity at concentrations of 0.1-1.0 wt%, indicating good biocompatibility of the polymers. CONCLUSIONS: The resultant thiolated hexanoyl glycol chitosans may play a crucial role in mucoadhesive applications in biomedical areas.

14.
Nano Lett ; 18(4): 2316-2323, 2018 04 11.
Artigo em Inglês | MEDLINE | ID: mdl-29561626

RESUMO

Monolayer (1L) transition metal dichalcogenides (TMDCs) are promising materials for nanoscale optoelectronic devices because of their direct band gap and wide absorption range (ultraviolet to infrared). However, 1L-TMDCs cannot be easily utilized for practical optoelectronic device applications (e.g., photodetectors, solar cells, and light-emitting diodes) because of their extremely low optical quantum yields (QYs). In this investigation, a high-gain 1L-MoS2 photodetector was successfully realized, based on the surface plasmon (SP) of the Ag nanowire (NW) network. Through systematic optical characterization of the hybrid structure consisting of a 1L-MoS2 and the Ag NW network, it was determined that a strong SP and strain relaxation effect influenced a greatly enhanced optical QY. The photoluminescence (PL) emission was drastically increased by a factor of 560, and the main peak was shifted to the neutral exciton of 1L-MoS2. Consequently, the overall photocurrent of the hybrid 1L-MoS2 photodetector was observed to be 250 times better than that of the pristine 1L-MoS2 photodetector. In addition, the photoresponsivity and photodetectivity of the hybrid photodetector were effectively improved by a factor of ∼1000. This study provides a new approach for realizing highly efficient optoelectronic devices based on TMDCs.

15.
ACS Appl Mater Interfaces ; 10(12): 10322-10329, 2018 Mar 28.
Artigo em Inglês | MEDLINE | ID: mdl-29508611

RESUMO

Hybrid structures of two-dimensional (2D) materials and quantum dots (QDs) are particularly interesting in the field of nanoscale optoelectronic devices because QDs are efficient light absorbers and can inject photocarriers into thin layers of 2D transition-metal dichalcogenides, which have high carrier mobility. In this study, we present a heterostructure that consists of a monolayer of tungsten diselenide (ML WSe2) covered by nitrogen-doped graphene QDs (N-GQDs). The improved photoluminescence of ML WSe2 is attributed to the dominant neutral exciton emission caused by the n-doping effect. Owing to strong light absorption and charge transfer from N-GQDs to ML WSe2, N-GQD-covered ML WSe2 showed up to 480% higher photoresponsivity than that of a pristine ML WSe2 photodetector. The hybrid photodetector exhibits good environmental stability, with 46% performance retention after 30 days under ambient conditions. The photogating effect also plays a key role in the improvement of hybrid photodetector performance. On applying the back-gate voltage modulation, the hybrid photodetector shows a responsivity of 2578 A W-1, which is much higher than that of the ML WSe2-based device.

16.
Polymers (Basel) ; 10(8)2018 Jul 30.
Artigo em Inglês | MEDLINE | ID: mdl-30960764

RESUMO

Adipose-derived mesenchymal stem cells (AD-MSCs) have been studied as desirable cell sources for regenerative medicine and therapeutic application. However, it has still remained a challenge to obtain enough adequate and healthy cells in large quantities. To overcome this limitation, various biomaterials have been used to promote expansion of MSCs in vitro. Recently, hexanoyl glycol chitosan (HGC) was introduced as a new biomaterial for various biomedical applications, in particular 3D cell culture, because of its biodegradability, biocompatibility, and other promising biofunctional properties. In this study, the effect of HGC on the proliferation of AD-MSCs was examined in vitro, and its synergistic effect with basic fibroblast growth factor (bFGF), which has been widely used to promote proliferation of cells, was evaluated. We found that the presence of HGC increased the proliferative capacity of AD-MSCs during long-term culture, even at low concentrations of bFGF. Furthermore, it suppressed the expression of senescence-related genes and improved the mitochondrial functionality. Taken all together, these findings suggest that the HGC demonstrate a potential for sustained growth of AD-MSCs in vitro.

17.
J Food Prot ; 80(11): 1842-1850, 2017 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-28990821

RESUMO

Although campylobacteriosis caused by Campylobacter jejuni and Campylobacter coli has been increasingly reported worldwide owing to the consumption of contaminated poultry and fresh produce, the current detection protocols are not selective enough to inhibit unspecific microbes other than these pathogens. Five antibiotics were separately added to Bolton broth, and the survival rates of 18 Campylobacter spp. and 79 non-Campylobacter spp. were evaluated. The survival rate of the non-Campylobacter spp. was the lowest in Bolton broth with rifampin (6.3%), followed by cefsulodin (12.7%), novobiocin (16.5%), and potassium tellurite and sulfamethozaxole (both 17.7%). Also the most effective concentration of rifampin was found to be 12.5 mg/L, which markedly inhibited non-Campylobacter strains while not affecting the survival of Campylobacter strains. After the Campylobacter spp. were enriched in Bolton broth supplemented with 12.5 mg/L rifampin (R-Bolton broth), CampyFood Agar (CFA) was found to be better in selectively isolating the pathogens in the enrichment broth than the International Organization for Standardization method of using modified charcoal cefoperazone deoxycholate agar (mCCDA) for this step. When applied to natural food samples-here, romaine lettuce, pepper, cherry tomato, Korean leek, and chicken-the R-Bolton broth-CFA combination decreased the number of false-positive results by 50.0, 4.2, 20.8, 50.0, and 94.4%, respectively, compared with the International Organization for Standardization method (Bolton broth-mCCDA combination). These results demonstrate that the combination of R-Bolton broth and CFA is more efficient in detecting C. jejuni and C. coli in poultry and fresh produce and thus should replace the Bolton broth-mCCDA combination.

18.
Adv Mater ; 29(18)2017 May.
Artigo em Inglês | MEDLINE | ID: mdl-28262993

RESUMO

This paper reports on the integration of freestanding transition metal dichalcogenides (TMDs). Monolayer (1-L) MoS2 , WS2 , and WSe2 as representative TMDs are transferred on ZnO nanorods (NRs), used here as nanostructured substrates. The photoluminescence (PL) spectra of 1-L TMDs on NRs show a giant PL intensity enhancement, compared with those of 1-L TMDs on SiO2 . The strong increases in Raman and PL intensities, along with the characteristic peak shifts, confirm the absence of stress in the TMDs on NRs. In depth analysis of the PL emission also reveals that the ratio between the exciton and trion peak intensity is almost not modified after transfer. The latter shows that the effect of charge transfer between the 1-L TMDs and ZnO NRs is here negligible. Furthermore, confocal PL and Raman spectroscopy reveal a fairly consistent distribution of PL and Raman intensities. These observations are in agreement with a very limited points contact between the support and the 1-L TMDs. The entire process reported here is scalable and may pave the way for the development of very efficient ultrathin optoelectronics.

19.
ACS Nano ; 10(11): 10446-10453, 2016 11 22.
Artigo em Inglês | MEDLINE | ID: mdl-27783894

RESUMO

Modulation of the carrier concentration and electronic type of monolayer (1L) MoS2 is highly important for applications in logic circuits, solar cells, and light-emitting diodes. Here, we demonstrate the tuning of the electronic properties of large-area 1L-MoS2 using graphene oxide (GO). GO sheets are well-known as hole injection layers since they contain electron-withdrawing groups such as carboxyl, hydroxyl, and epoxy. The optical and electronic properties of GO-treated 1L-MoS2 are dramatically changed. The photoluminescence intensity of GO-treated 1L-MoS2 is increases by more than 470% compared to the pristine sample because of the increase in neutral exciton contribution. In addition, the A1g peak in Raman spectra shifts considerably, revealing that GO treatment led to the formation of p-type doped 1L-MoS2. Moreover, the current vs voltage (I-V) curves of GO-coated 1L-MoS2 field effect transistors show that the electron concentration of 1L-MoS2 is significantly lower in comparison with pristine 1L-MoS2. Current rectification is also observed from the I-V curve of the lateral diode structure with 1L-MoS2 and 1L-MoS2/GO, indicating that the electronic structure of MoS2 is significantly modulated by the electron-withdrawing functional group of GO.

20.
ACS Appl Mater Interfaces ; 8(45): 31222-31230, 2016 Nov 16.
Artigo em Inglês | MEDLINE | ID: mdl-27778509

RESUMO

Despite recent progress in producing flexible and stretchable electronics based on two-dimensional (2D) nanosheets, their intrinsic properties are often degraded by the presence of polymeric residues that remain attached to the 2D nanosheet surfaces following fabrication. Further breakthroughs are therefore keenly awaited to obtain clean surfaces compatible with flexible applications. Here, we report a method that allows the 2D nanosheets to be intrinsically integrated onto flexible substrates. The method involves thermal decomposition of polymeric residues by microwave-induced ultrafast heating of the surface without affecting the underlying flexible substrate. Mapping the C═O stretching mode by Fourier-transform infrared spectroscopy in combination with atomic force microscopy confirms elimination of the polymeric residues from the 2D nanosheet surface. Flexible devices prepared using microwave-cleaned 2D nanosheets show enhanced electrical, optical, and electrothermal performances. This simple technique is applicable to a wide range of 2D nanomaterials and represents an important advance in the field of flexible devices.

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