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13 result(s) for "Chou, Ho-Hsiu"
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A skin-inspired organic digital mechanoreceptor
Human skin relies on cutaneous receptors that output digital signals for tactile sensing in which the intensity of stimulation is converted to a series of voltage pulses. We present a power-efficient skin-inspired mechanoreceptor with a flexible organic transistor circuit that transduces pressure into digital frequency signals directly. The output frequency ranges between 0 and 200 hertz, with a sublinear response to increasing force stimuli that mimics slow-adapting skin mechanoreceptors. The output of the sensors was further used to stimulate optogenetically engineered mouse somatosensory neurons of mouse cortex in vitro, achieving stimulated pulses in accordance with pressure levels. This work represents a step toward the design and use of large-area organic electronic skins with neural-integrated touch feedback for replacement limbs.
Overcoming small-bandgap charge recombination in visible and NIR-light-driven hydrogen evolution by engineering the polymer photocatalyst structure
Designing an organic polymer photocatalyst for efficient hydrogen evolution with visible and near-infrared (NIR) light activity is still a major challenge. Unlike the common behavior of gradually increasing the charge recombination while shrinking the bandgap, we present here a series of polymer nanoparticles (Pdots) based on ITIC and BTIC units with different π-linkers between the acceptor-donor-acceptor (A-D-A) repeated moieties of the polymer. These polymers act as an efficient single polymer photocatalyst for H2 evolution under both visible and NIR light, without combining or hybridizing with other materials. Importantly, the difluorothiophene (ThF) π-linker facilitates the charge transfer between acceptors of different repeated moieties (A-D-A-(π-Linker)-A-D-A), leading to the enhancement of charge separation between D and A. As a result, the PITIC-ThF Pdots exhibit superior hydrogen evolution rates of 279 µmol/h and 20.5 µmol/h with visible (>420 nm) and NIR (>780 nm) light irradiation, respectively. Furthermore, PITIC-ThF Pdots exhibit a promising apparent quantum yield (AQY) at 700 nm (4.76%). Designing an organic polymer photocatalyst for efficient hydrogen evolution in the near-infrared (NIR) light region is still a major challenge. The authors present here a series of polymer nanoparticles for a efficient hydrogen evolution under visible and NIR light irradiation, without combining or hybridizing with other materials.
Main-chain engineering of polymer photocatalysts with hydrophilic non-conjugated segments for visible-light-driven hydrogen evolution
Photocatalytic water splitting is attracting considerable interest because it enables the conversion of solar energy into hydrogen for use as a zero-emission fuel or chemical feedstock. Herein, we present a universal approach for inserting hydrophilic non-conjugated segments into the main-chain of conjugated polymers to produce a series of discontinuously conjugated polymer photocatalysts. Water can effectively be brought into the interior through these hydrophilic non-conjugated segments, resulting in effective water/polymer interfaces inside the bulk discontinuously conjugated polymers in both thin-film and solution. Discontinuously conjugated polymer with 10 mol% hexaethylene glycol-based hydrophilic segments achieves an apparent quantum yield of 17.82% under 460 nm monochromatic light irradiation in solution and a hydrogen evolution rate of 16.8 mmol m −2 h −1 in thin-film. Molecular dynamics simulations show a trend similar to that in experiments, corroborating that main-chain engineering increases the possibility of a water/polymer interaction. By introducing non-conjugated hydrophilic segments, the effective conjugation length is not altered, allowing discontinuously conjugated polymers to remain efficient photocatalysis. The introduction of hydrophilic segments into the main-chain of polymer photocatalysts allows water to efficiently enter the interior through these hydrophilic segments, and results in effective water/polymer interfaces for hydrogen evolution.
Construction of Porous Organic/Inorganic Hybrid Polymers Based on Polyhedral Oligomeric Silsesquioxane for Energy Storage and Hydrogen Production from Water
In this study, we used effective and one-pot Heck coupling reactions under moderate reaction conditions to construct two new hybrid porous polymers (named OVS-P-TPA and OVS-P-F HPPs) with high yield, based on silsesquioxane cage nanoparticles through the reaction of octavinylsilsesquioxane (OVS) with different brominated pyrene (P-Br4), triphenylamine (TPA-Br3), and fluorene (F-Br2) as co-monomer units. The successful syntheses of both OVS-HPPs were tested using various instruments, such as X-ray photoelectron (XPS), solid-state 13C NMR, and Fourier transform infrared spectroscopy (FTIR) analyses. All spectroscopic data confirmed the successful incorporation and linkage of P, TPA, and F units into the POSS cage in order to form porous OVS-HPP materials. In addition, the thermogravimetric analysis (TGA) and N2 adsorption analyses revealed the thermal stabilities of OVS-P-F HPP (Td10 = 444 °C; char yield: 79 wt%), with a significant specific surface area of 375 m2 g–1 and a large pore volume of 0.69 cm3 g–1. According to electrochemical three-electrode performance, the OVS-P-F HPP precursor displayed superior capacitances of 292 F g−1 with a capacity retention of 99.8% compared to OVS-P-TPA HPP material. Interestingly, the OVS-P-TPA HPP showed a promising HER value of 701.9 µmol g−1 h−1, which is more than 12 times higher than that of OVS-P-F HPP (56.6 µmol g−1 h−1), based on photocatalytic experimental results.
A chameleon-inspired stretchable electronic skin with interactive colour changing controlled by tactile sensing
Some animals, such as the chameleon and cephalopod, have the remarkable capability to change their skin colour. This unique characteristic has long inspired scientists to develop materials and devices to mimic such a function. However, it requires the complex integration of stretchability, colour-changing and tactile sensing. Here we show an all-solution processed chameleon-inspired stretchable electronic skin (e-skin), in which the e-skin colour can easily be controlled through varying the applied pressure along with the applied pressure duration. As such, the e-skin’s colour change can also be in turn utilized to distinguish the pressure applied. The integration of the stretchable, highly tunable resistive pressure sensor and the fully stretchable organic electrochromic device enables the demonstration of a stretchable electrochromically active e-skin with tactile-sensing control. This system will have wide range applications such as interactive wearable devices, artificial prosthetics and smart robots. Some animals and insects can change the colour of their skin, but mimicking such function in man-made materials is complex. Here, the authors demonstrate an all-solution processed chameleon-inspired stretchable e-skin capable of interactive colour changes and tactile sensing.
Mechanistic Studies of Hydrogen Evolution Reaction on Donor-Acceptor Conjugated Polymer Photocatalysts
The application of donor-acceptor (D-A) conjugated polymer catalysts for hydrogen evolution reaction (HER) has shown great promise because of the tunability of such catalysts to have desired properties. Herein, we synthesized two polymer catalysts: poly[4,4′-(9-(4-aminophenyl)-9H-carbazole-3,6-diamine-alt-5-oxido-5-phenylbenzo[b]phosphindole-3,7-diyl)dibenzaldehyde] (PCzPO) and poly[N1,N1-bis(4-amino-2-fluorophenyl)-2-fluorobenzene-1,4-diamine-alt-5-oxido-5-phenylbenzo[b]phosphindole-3,7-diyl)dibenzaldehyde] (PNoFPO). The UV-vis absorption spectra showed that the less planar structure and the presence of electronegative fluorine atoms in the donor group of PNoFPO led to a higher optical gap compared to PCzPO, leading to almost five times faster HER rate using PCzPO compared to PNoFPO. However, density functional theory (DFT) calculations show that the frontier orbitals and the highest occupied molecular orbitals – lowest unoccupied molecular orbitals (HOMO-LUMO) gaps of PCzPO and PNoFPO D-A moiety models are very similar, such that, during light absorption, electrons move from donor to acceptor group where proton binding is preferred to happen thereafter. For both PCzPO and PNoFPO D-A moieties, H2 formation through an intramolecular reaction with a barrier of 0.6–0.7 eV, likely occurs at the acceptor group atoms where protons bind through electrostatic interaction. The intermolecular reaction has nearly zero activation energy but is expected to occur only when the repulsion is low between separate polymers chains. Finally, experimental and DFT results reveal the importance of extended configurations of D-A polymers on HER rate.
Solar-driven photocatalytic hydrogen production thiophene-quinoxaline-based polymer dots with tunable molecular weight
Organic conjugated polymer dots (Pdots) are considered promising photocatalysts for solar-driven hydrogen production. However, the impact of molecular weight on their photocatalytic activity remains unexplored. In this study, four thiophene-quinoxaline (PTQ)-based Pdots (D-A system) with tunable molecular weights were fabricated to elucidate the effects of molecular weight on Pdot photocatalytic activity. These Pdots serve as highly efficient and stable photocatalysts for visible-light-driven hydrogen generation in a solvent-free organic system, which was achieved for the first time. Low-molecular-weight Pdots exhibited minimal aggregation, small particle sizes, uniform morphology, enhanced charge transfer capability, and superior photocatalytic activity with remarkable photostability. Notably, L-PTQ10 and L-PTQ11 demonstrated exceptional hydrogen evolution rates of 15,807 and 10,411 μmol g−¹ h−¹, respectively, when coupled with a Pt cocatalyst. The findings from our DFT and molecular dynamics (MD) calculations strongly support our hypothesis, highlighting the use of low-molecular-weight PTQ-based Pdots as a promising strategy to develop efficient and stable photocatalysts for solar-driven hydrogen production.This study presents the synthesis of thiophene-quinoxaline (PTQ)-based polymer dots (Pdots) with tunable molecular weights (D-A system) for the first time. Remarkably, Low-molecular weight Pdots exhibit minimal aggregation, small size, and enhanced charge transfer, leading to superior photocatalytic activity and remarkable photostability.
Effective remediation of Pb2+ polluted environment by adsorption onto recyclable hydroxyl bearing covalent organic framework
The removal of heavy metal ions from wastewater has attracted considerable interest because of their toxicity. Adsorption is one of the most promising methods for the removal of heavy metal ions due to its simplicity and effectiveness. Recently, covalent organic frameworks (COFs) have become promising adsorbents for effective wastewater remediation. However, many building blocks have been developed, and the design of COFs with high adsorption efficiency remains a challenge. Here, a covalent organic framework (DHTP-TPB COF) decorated with hydroxyl groups was developed for the efficient removal of Pb 2+ ions. The DHTP-TPB COF showed excellent performance in adsorbing Pb 2+ from aqueous solution. More importantly, DHTP-TPB COF exhibited high selectivity for Pb 2+ compared to other competing ions, capturing Pb 2+ ions with a removal efficiency of over 96% at pH 4. The results show that the DHTP-TPB COF exhibits excellent adsorption capacity at pH 4 of up to 154.3 mg/g for Pb 2+ ions; the value is comparable to many previously reported COFs. Moreover, the adsorbed Pb 2+ ions could be easily eluted with a 0.1 M EDTA solution, and the DHTP-TPB COF can be reused for more than five adsorption–desorption cycles without significant loss of adsorption capacity. Moreover, the adsorption mechanism was revealed using XPS analysis, indicating the formation of strong coordination-bonding interactions between hydroxyl and Pb 2+ ions. Therefore, the DHTP-TPB COF prepared herein has high potential for the treatment of Pb 2+ -contaminated wastewater and is promising for the adsorption of Pb 2+ ions in practical applications. Graphical Abstract
Effective remediation of Pb 2+ polluted environment by adsorption onto recyclable hydroxyl bearing covalent organic framework
The removal of heavy metal ions from wastewater has attracted considerable interest because of their toxicity. Adsorption is one of the most promising methods for the removal of heavy metal ions due to its simplicity and effectiveness. Recently, covalent organic frameworks (COFs) have become promising adsorbents for effective wastewater remediation. However, many building blocks have been developed, and the design of COFs with high adsorption efficiency remains a challenge. Here, a covalent organic framework (DHTP-TPB COF) decorated with hydroxyl groups was developed for the efficient removal of Pb ions. The DHTP-TPB COF showed excellent performance in adsorbing Pb from aqueous solution. More importantly, DHTP-TPB COF exhibited high selectivity for Pb compared to other competing ions, capturing Pb ions with a removal efficiency of over 96% at pH 4. The results show that the DHTP-TPB COF exhibits excellent adsorption capacity at pH 4 of up to 154.3 mg/g for Pb ions; the value is comparable to many previously reported COFs. Moreover, the adsorbed Pb ions could be easily eluted with a 0.1 M EDTA solution, and the DHTP-TPB COF can be reused for more than five adsorption-desorption cycles without significant loss of adsorption capacity. Moreover, the adsorption mechanism was revealed using XPS analysis, indicating the formation of strong coordination-bonding interactions between hydroxyl and Pb ions. Therefore, the DHTP-TPB COF prepared herein has high potential for the treatment of Pb -contaminated wastewater and is promising for the adsorption of Pb ions in practical applications.