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1.
Adv Mater ; 35(44): e2304694, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-37660286

RESUMO

Covalently functionalized germanane is a novel type of fluorescent probe that can be employed in material science and analytical sensing. Here, a fluorometric sensing platform based on methyl-functionalized germanane (CH3 Ge) is developed for gas (humidity and ammonia) sensing, pH (1-9) sensing, and anti-counterfeiting. Luminescence (red-orange) is seen when a gas molecule intercalates into the interlayer space of CH3 Ge and the luminescence disappears upon deintercalation. This allows for direct detection of gas absorption via fluorometric measurements of the CH3 Ge. Structural and optical properties of CH3 Ge with intercalated gas molecules are investigated by density functional theory (DFT). To demonstrate real-time and on-the-spot testing, absorbed gas molecules are first precisely quantified by CH3 Ge using a smartphone camera with an installed color intensity processing application (APP). Further, CH3 Ge-paper-based sensor is integrated into real food packets (e.g., fish and milk) to monitor the shelf life of perishable foods. Finally, CH3 Ge-based rewritable paper is applied in water jet printing to illustrate the potential for secret communication with quick coloration and good reversibility by water evaporation.

2.
ACS Appl Mater Interfaces ; 13(18): 21426-21435, 2021 May 12.
Artigo em Inglês | MEDLINE | ID: mdl-33938731

RESUMO

Rechargeable aqueous zinc-iodine batteries (AZIBs) represent excellent zinc-iodine redox chemistry and emerged as a promising aspirant due to their high safety, low cost, ease of fabrication, and high energy density. Nevertheless, the high-dissolution-induced iodide diffusion toward the zinc anode brings the self-discharge, which governs the capacity fading and poor cycling life of the battery. Herein, a multipurpose sponge-like porous matrix of a metal-organic gel to host a substantial amount of an iodine-based catholyte and uniform distribution of iodine with controlled iodide diffusion is introduced. Limiting the iodine diffusion due to increased viscosity provides superior electrochemical performance of this promising cathode for solid-state AZIBs. As a result, AZIBs delivering high performance and long-term stability are fabricated with a capacity of 184.9 mA h g-1 with a superior capacity retention of 95.8% even after 1500 cycles at 1 C rate. The unique concept of self-discharge protection is successfully evaluated. Prototype flexible band-aid-type AZIBs were fabricated, which delivered 166.4 mA h g-1 capacity in the bending state, and applied to real-scale wearable applications.

3.
ACS Appl Mater Interfaces ; 12(20): 22939-22947, 2020 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-32319745

RESUMO

Here, we report phosphonium-based two solid ionic conductors (SICs), namely, triphenylphosphonium methyl iodide (TPPMeI) and triphenylphosphonium iodide (TPPHI), prepared via simple protocol at room temperature and were used as an electrolyte for solid-state photovoltaic devices (ss-PVDs) with open-circuit voltage (Voc) exceeding 800 mV. Here, for the first time, detailed electrochemical investigations with theoretical aspects of phosphonium electrolytes were conducted, where PVDs prepared from these SICs, TPPMeI, showed the highest power conversion efficiency (PCE) of 4.08% with a Voc of 810 mV. However, this performance was further improved up to the PCE of 6.71% with 824 mV of Voc in the presence of additives like LiI and tert-butyl pyridine. This work leads to find the best alternative of liquid and quaternary ammonium ion-based electrolytes that suffers from problems like lower Voc (<800 mV) and stability, leakage, etc.

4.
Small ; 14(36): e1800842, 2018 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-30091844

RESUMO

Quasi-solid-state dye-sensitized solar cells (DSSCs) fabricated with lightweight flexible substrates have a great potential in wearable electronic devices for in situ powering. However, the poor lifespan of these DSSCs limits their practical application. Strong mechanical stresses involved in practical applications cause breakage of the electrode/electrolyte interface in the DSSCs greatly affecting their performance and lifetime. Here, a mechanically robust, low-cost, long-lasting, and environment-friendly quasi-solid-state DSSC using a smart thermoreversible water-based polymer gel electrolyte with self-healing characteristics at a low temperature (below 0 °C) is demonstrated. When the performance of the flexible DSSC is hindered by strong mechanical stresses (i.e., from multiple bending/twisting/shrinking actions), a simple cooling treatment can regenerate the electrode/electrolyte interface and recover the performance close to the initial level. A performance recovery as high as 94% is proven possible even after 300 cycles of 90° bending. To the best of our knowledge, this is the first aqueous DSSC device with self-healing behavior, using a smart thermoreversible polymer gel electrolyte, which provides a new perspective in flexible wearable solid-state photovoltaic devices.

5.
Phys Chem Chem Phys ; 19(42): 28579-28587, 2017 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-29058011

RESUMO

The preparation of a series of organic dyes having a carbazole donor, cyanoacrylic acid as an acceptor, and phenylene ring as a spacer with the difference in the positions of fluorine substitution is reported. Due to its unique properties of small size and high electronegativity, fluorine is now being extensively used to control the optoelectronic properties of organic conjugated materials. In this study, the results revealed that the specific position and number of fluorine substitution were very crucial to control the optical as well as the electrochemical properties of organic dyes. It was found that fluorine substitution led to a redshift in the absorption spectra of the dyes and reduced the band gap. The injection rate of photoexcited electrons was measured using time-resolved photoluminescence and the o-fluoro substituted dye MA1F-o showed the best electron injection dynamics. As a result of broad absorption and high electron injection rate, the dye MA1F-o outperformed other dyes with a power conversion efficiency of 4.02% (Jsc = 8.3 mA cm-2, Voc = 0.75 V and FF = 0.64). The non-fluorinated dye MA0F exhibited a power conversion efficiency of 3.23% (Jsc = 6.8, Voc = 0.72 and FF = 0.67). The dye MA1F-m exhibited the least molar absorption coefficient and a lower power conversion efficiency because of the meta inductive effect.

6.
Nanoscale ; 9(41): 15949-15957, 2017 Oct 26.
Artigo em Inglês | MEDLINE | ID: mdl-29019499

RESUMO

A novel saturated heterocyclic organic ionic crystal, piperidinium iodide (PiHI), is synthesized by a facile route and applied as a solid electrolyte in Dye Sensitized Solar Cells (ss-DSSCs). Upon addition of a small quantity of iodine, PiHI self-assembles into a 1D lamellar micro crystalline structure that shows anisotropic conductivity. The two-component PiHI was characterized by using electrochemical impedance spectroscopy, cyclic voltammetry, steady state voltammetry, FT-IR, and Raman spectroscopy. Wide angle X-ray diffraction (XRD) measurement confirms the presence of long range 1D lamellar channels that pave the way for the diffusion of the redox couple I-/I3- and exhibit high anisotropic conductivity. The ionic conductivity of 1D PiHI (with I2) aligned perpendicular to the electrode, σ⊥ (15.46 mS cm-1), is 1.5 times higher than that aligned parallel to the electrode σ∥ = 10.32 mS cm-1. The ss-DSSC devices with these self-assembled ordered ionic crystals with a carbazole based sensitizer (SK1) achieved a power conversion efficiency (PCE) of 4.2% and 5.2% for ∥al and ⊥ar arrangement, respectively. The reported PCEs are better than that obtained from a classical liquid electrolyte with SK1 sensitizers. The electron kinetics at various interfaces of ss-DSSC devices was evaluated using Electrochemical Impedance Spectroscopy (EIS) measurements. The presence of a saturated cyclic structure promotes close packing through H-bonding and electrostatic interactions, which make ss-DSSC devices more stable up to 600 h under illumination of 1 sun.

7.
Angew Chem Int Ed Engl ; 56(27): 7871-7875, 2017 06 26.
Artigo em Inglês | MEDLINE | ID: mdl-28503917

RESUMO

Flexible batteries are essential for wearable electronic devices. To meet practical applications, they need to be mechanically robust and stable. However, strong or multiple bending may sever the interfacial contact between electrode and electrolyte, causing capacity fading or even battery failure. Herein we present a new cooling-recovery concept for flexible batteries, which involves a temperature-sensitive sol-gel transition behavior of the thermoreversible polymer hydrogel electrolyte. Once a battery has suffered from strong mechanical stresses, a simple cooling process can refresh the electrode-electrolyte interface. The energy-storage capability can be recovered with a healing efficiency higher than 98 %. It is believed that this study not only offers new valuable insights, but also opens up new perspectives to develop functional wearable devices.

8.
ACS Omega ; 1(1): 14-18, 2016 Jul 31.
Artigo em Inglês | MEDLINE | ID: mdl-31457114

RESUMO

Humic acid (HA), a natural polymer and soil component, was explored as a photosensitizer in dye-sensitized solar cells (DSSCs). Photophysical and electrochemical properties show that HA covers a broad visible range of the electromagnetic spectrum and exhibits a quasi-reversible nature in cyclic voltammetry (CV). Because of its abundant functionalities, HA was able to bind onto the nano-titania surface and possessed good thermal stability. HA was employed as a sensitizer in DSSCs and characterized by various photovoltaic techniques such as I-V, incident-photo-to-current conversion efficiency (IPCE), electrochemical impedance spectroscopy (EIS), and Tafel polarization. The HA-based device shows a power conversion efficiency (PCE) of 1.4% under 1 sun illumination. The device performance was enhanced when a coadsorbent, chenodeoxycholic acid (CDCA), along with HA was used and displayed 2.4% PCE under 0.5 sun illumination. The DSSCs employing HA with CDCA showed excellent stability up to 1000 h. The reported efficiency of devices with HA is better than that of devices with all natural sensitizers reported so far.

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